Review

ChemPhysChem doi.org/10.1002/cphc.202400459

www.chemphyschem.org

Life Cycle of LiFePO4 Batteries: Production, Recycling, and

Market Trends
Hossein Rostami,*[a, b] Johanna Valio,[b] Pekka Tynjälä,[a, c] Ulla Lassi,[a, c] and Pekka Suominen[b]

Significant attention has focused on olivine-structured LiFePO4 the depletion of valuable resources
(LFP) as a promising cathode active material (CAM) for lithium- This review comprehensively examines diverse synthesis ap-
ion batteries. This iron-based compound offers advantages over proaches for generating LFP powders, encompassing conven-
commonly used Co and Ni due to its lower toxicity abundance, tional methodologies alongside novel procedures. Furthermore,
and cost-effectiveness. Despite its current commercial use in it conducts an in-depth assessment of the methodologies
energy storage technology, there remains a need for cost- employed in recycling waste LFP batteries. Moreover, it
effective production methods to create electrochemically active emphasizes the importance of LFP cathode recycling and
LiFePO4. Consequently, there is ongoing interest in developing investigates pretreatment techniques to enhance understand-
innovative approaches for LiFePO4 production. While LFP ing. Additionally, it provides valuable insights into the recycling
batteries exhibit significant thermal stability, cycling perform- process of used LFP batteries, aiming to raise awareness
ance, and environmental benefits, their growing adoption has regarding the market for retired LFP batteries and advocate for
increased battery disposal rates. Improper disposal practices for the enduring sustainability of lithium-ion batteries.
waste LFP batteries result in environmental degradation and

1. Introduction olivine crystal structure occurs along one-dimensional channels,

with limited opportunities for crossing between these channels.
The olivine structure of LiFePO4 (LFP) has a hexagonally close- These narrow pathways are especially prone to blockage by
packed oxygen array in which the octahedra share both edges defects and impurities.[2,3] Several strategies have been inves-
and faces (Figure 1a). The arrangement of cations in LiFePO4 tigated to mitigate the conductivity challenge, such as
differs notably from that in layered and spinel structures like diminishing particle dimensions and achieving uniformity in
LCO and LMO, respectively. Unlike these structures, LiFePO4 particle size distribution,[4] coating the particles with carbon,[5,6]
lacks a continuous network of FeO6 edge-shared octahedra that or synthesizing compounds with carbon to envelop each
could enhance electronic conductivity. LiFePO4 has emerged as particle with a proficient electronic conductor,[7] Tailoring the
a top positive electrode material in the past decade thanks to a morphology and texture of the particle through low-temper-
deep understanding of its structural changes during lithium ature synthesis routes,[8] and selective doping with cations to
insertion and clever manipulation of particle shapes. Based on increase the intrinsic conductivity.
this one-electron process, 170 mAh g 1 is the theoretical The demand for LFP batteries as energy storage devices has
capacity. However, because of electron and ion transport significantly increased due to their notable advantages, includ-
restrictions, early attempts to remove Li from this material were ing long lifespan, enhanced discharge and charge efficiency,
only able to remove around 0.6 e .[1] The primary hurdle to and safe usage. Furthermore, the appeal of LFP batteries is
achieving the theoretical capacity of LiFePO4 is its low inherent further strengthened by the limited availability of critical raw
electronic conductivity. Also, lithium movement within the materials for NMC batteries and their cost-effectiveness, leading
to a surge in demand for LFP batteries. The rise in the
[a] H. Rostami, P. Tynjälä, U. Lassi production of high-energy storage devices, electric vehicles
University of Oulu, Research Unit of Sustainable Chemistry, P.O.Box 3000, (EVs), and hybrid electric vehicles (HEVs) has resulted in a
FI-90014 Oulu, Finland significant surge in the utilization of LFP batteries.[9] Indeed, the
E-mail: [email protected] widespread utilization of LFP batteries elicits dual concerns
[b] H. Rostami, J. Valio, P. Suominen
surrounding their impact on the economy and the environ-
Satakunta University of Applied Sciences (SAMK), Satakunnankatu 23, FI-
28130 Pori, Finland ment. The high extraction costs and unpredictable product
[c] P. Tynjälä, U. Lassi quality associated with lithium production for LFP synthesis
University of Jyvaskyla, Kokkola University Consortium Chydenius, Talonpo- provide economic challenges. The extensive consumption of
jankatu 2B, FI-67100 Kokkola, Finland LFP batteries may lead to a significant issue in the future, as
Supporting information for this article is available on the WWW under many spent batteries accumulate despite their current opera-
https://doi.org/10.1002/cphc.202400459
tional lifespan.[10] Therefore, recycling these batteries aids in
© 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH. This is
preventing environmental pollution and reclaiming valuable
an open access article under the terms of the Creative Commons Attribution
License, which permits use, distribution and reproduction in any medium, materials for reuse.
provided the original work is properly cited.

ChemPhysChem 2024, 25, e202400459 (1 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

This review introduces the current state of recycling for 2. Synthesis of LFP
spent LFP batteries and analyzes various recycling technologies.
Additionally, it summarizes the latest advancements in novel Since John Goodenough discovered the olivine phase’s electro-
methods developed in recent years. Up until now, the recycling chemical characteristics in 1997, numerous synthesis routes of
of spent LFP batteries has mainly been carried out using two the olivine-type LiFePO4 were explored.[11] A general distinction
traditional methods: (1) pyrometallurgy (i. e., direct regenera- can be made between processes that start in the solid phase
tion) and (2) hydrometallurgy (i. e., the leaching of individual and those that commence in the solution phase.
metals). This review outlines the procedures for synthesizing The synthesis of lithium iron phosphate can be achieved
(doped and coated) LFP powders, starting from the necessary through solid-phase or liquid-phase methods. Solid phase
raw materials. Alongside established traditional synthesis routes techniques like high-temperature reactions, carbothermal re-
for LFP, it discusses various alternative methods. It also duction, and microwave synthesis are favored for their
examines the properties of LFP and introduces essential raw simplicity and suitability for industrial production. Lithium iron
materials for LFP within the battery value chain. Also, the review phosphate is coated with pyrolytic carbon to enhance con-
addresses the limited coverage of recycling technologies for ductivity in the carbothermal reduction method. Liquid phase
spent LFP batteries, which often concentrate on conventional methods such as precipitation, sol-gel, and hydrothermal syn-
methods or singular recovery approaches. It highlights critical thesis, offer uniform mixing and better product consistency but
recycling techniques for LFP cathodes and provides an overview require high-pressure, high-temperature conditions, and com-
of pretreatment technologies to enhance comprehension. plex equipment, making mass production challenging. Fig-
Moreover, it offers insights into the development of spent LFP ure 1b compares the solid-phase and liquid-phase synthesis
recycling, aiming to draw attention to the retired LFP market methods.
and promote the long-term sustainability of lithium-ion
batteries.

Hossein Rostami holds a Ph.D. in electro- tions and five patents. He has been an
chemistry from the University of Mazandaran entrepreneur for 14 years and has founded
(2016) and is currently a university researcher several start-up companies. Suominen has
at the University of Oulu, working in the been principal investigator in 10 research
Research Unit of Sustainable Chemistry. His projects.
research focuses on the synthesis of cathode
Pekka Tynjälä, Doctor of Philosophy (Univer-
materials for Li-ion batteries, as well as on
sity of Joensuu, 1998). He works as a university
coating, doping, battery cell preparation, and
researcher at the University of Oulu in the
various characterization techniques.
Research Unit of Sustainable Chemistry. His
research activities include hydrometallurgical
processes such as co-precipitation of lithium-
Johanna Valio holds a Master of Social ion battery precursor materials and leaching
Sciences in sociology from the University of of metallic materials in order to prepare
Joensuu (2003) and a Master of Science (Tech) battery-grade metal sulfate solutions.
in Chemical Engineering from Aalto University
(2017), specializing in Functional Materials.
Currently, Johanna Valio works as a researcher
SHORT CURRICULUM VITAE, Professor Ulla
at the RoboAI research centre, part of Sata-
Lassi
kunta University of Applied Sciences, and as a
Ulla Lassi, Doctor of Technology (2003),
principal investigator in AIST project (A novel
Professor at the University of Oulu in the
AI-based Spectroscopic Technique for recy-
Faculty of Technology (2006 ). She is also the
cling of battery materials). Her research inter-
Head of Research Unit of Sustainable
ests include holistic understanding of battery
Chemistry (67 employers). Her research areas
recycling.
involve inorganic material chemistry in indus-
Pekka Suominen, Doctor of Philosophy, trial applications, esp. catalysis and battery
Physics (2006 University of Jyväskylä), Head of chemicals. She has 230 scientific publications
Research in RoboAI research centre at Sata- and five patents. As a professor, she has
kunta University of Applied Sciences (25 supervised 30 PhD theses and 130 M.Sc the-
employers). His research interests are related ses. Lassi has been principal investigator of 40
to automation, robotics, artificial intelligence research projects. She has several positions of
and their industrial applications, especially in trust. Lassi has also been awarded Tandem
laser-induced breakdown spectroscopy and Industry Academy Professorship in battery
circular economy of technology metals and chemistry for 2023–2025.
battery materials. He has 45 scientific publica-

ChemPhysChem 2024, 25, e202400459 (2 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 1. (a) Schematic illustration of the olivine structure of LiFePO4, including FeO6 octahedra, PO4 tetrahedra, and Li + one-dimensional diffusion channel
and the phase transition process. Copyright 2023 Elsevier. Reproduced with permission from reference[12] and (b) Comparison of the process flow between
solid and liquid phase method for LFP synthesis.

2.1. Solid-State (Thermal) Synthesis of LFP heated at 300–400 °C in an inert atmosphere to decompose the
ligands. After regrinding, the powder is reheated at 400–800 °C
Solid-state synthesis is a traditional approach for producing for 10–24 h. Before the second grinding step, a carbon-
ceramics, involving multiple steps of thorough grinding and containing compound, such as carboxylic acid, can be added to
heating the precise mixture of starting materials. This mixture the precursor. This compound can serve as a carbon source in
typically comprises iron salt, such as Fe(II)-acetate or Fe(II)- the LiFePO4/C composite. The schematic presentation is given
oxalate, a lithium salt like lithium carbonate or lithium in Figure 2a.
hydroxide, and often includes ammonium phosphate as a The purity of the material relies on growth parameters such
source of phosphorus.[13–17] The reaction mixture is initially as calcination temperature and exposure time. During calcina-

ChemPhysChem 2024, 25, e202400459 (3 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 2. (a) Schematic illustration of solid-state synthesis for LFP, (b) TEM image of LiFePO4-PAS prepared at 700 °C for 4 h. Copyright 2008 Elsevier.
Reproduced with permission from reference[30] and (c) a planar diagram illustrating the process of microwave heating. Copyright 2021 Elsevier. Reproduced
with permission from reference.[27]

tion, an inert nitrogen or argon or slightly reductive atmosphere 2.1.1. Carbothermal Reduction
(argon or nitrogen with added hydrogen) is necessary due to
the iron oxidation state (+ 2). However, residual Fe3 + phase Low electronic conductivity is the main problem, which makes
presence is possible and frequently observed. Calcination above it challenging to use LiFePO4 as a battery cathode chemical in
800 °C results in the formation of both trivalent Fe2O3 and high-power applications such as HEVs. Several studies have
Li3Fe2(PO4)3. Trivalent Fe may form due to oxygen in the inert shown that the synthesis of LiFePO4 with a coating of an
gas flow or residual air trapped in particle pores. Another electronic conductor, such as a carbon layer, is an effective way
drawback of this method is uncontrollable particle size growth to increase the electrochemical properties of LiFePO4. The TEM
and agglomeration, limiting the application potential of larger image in Figure 2b shows how the carbon layer covers the
particles due to their small surface area. Despite being an LiFePO4 particles. Several studies have been done to determine
effective and easily industrialized method, the solid-state syn- the best process for synthesizing LiFePO4-C. Mi et al. have
thesis requires repeated reheating and regrinding to enhance presented a one-step process for synthesizing carbon-coated
final product homogeneity, rendering the processing time and LiFePO4 cathodes.[20] The starting mixture consists of stoichio-
energy-consuming.[13,17,18] Additionally, researchers have modi- metric amounts of inexpensive FePO4 ·4H2O and LiOH· H2O. The
fied traditional solid-state reactions, achieving LiFePO4 prepara- starting mixture was ball-milled for 2 h in a planetary mill with a
tion without using an inert gas flow. Researchers synthesized nylon vessel and then mixed with polypropylene as a carbon
the LiFePO4 by heating Fe2O3, NH4H2PO4, and LiOH in deionized source and reductive agent. The mixture was annealed at 650 °C
water for three hours at 700 °C.[19] for 10 h in a nitrogen atmosphere to synthesize carbon-coated
LiFePO4 powder.[20]
High-performance LiFePO4 cathode materials were pro-
duced through an advanced solid-state method utilizing starch

ChemPhysChem 2024, 25, e202400459 (4 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

and PEG6000 as a complex carbon source. The wet-mixing 2.2.1. Hydrothermal (Solvothermal) Synthesis
process in de-ionized water at 80 °C enhanced precursor
stabilization during drying and addressed challenges associated A fast, simple, cost-effective, energy-efficient, and easily scalable
with mixing in a water medium. The starch gelatinization at method for generating small particles is hydrothermal or
80 °C resulted in a gel emulsion precursor, which, after solvothermal synthesis. The synthesis of lithium iron phosphate
concentrated sedimentation during the drying process at via hydrothermal methods was initially demonstrated by mixing
120 °C, transformed into a compact dry gel. Finally, the obtained FeSO4, H3PO4, and LiOH in a molar ratio of 1 : 1 : 3. To prevent
dry gel was sintered at 700 °C for 12 h to yield the LiFePO4/C the formation of Fe(OH)2, which readily oxidizes to FeO(OH), the
composite.[21] A study presents an efficient supercritical CO2 FeSO4 and H3PO4 solution were initially combined. Then, LiOH
(SCCO2)-assisted ex-situ carbon-coating method for LFP. SCCO2 solution was added to the mixture, followed by hydrothermal
enhances carbon precursor penetration, yielding high-quality processing at 120 °C for up to 5 h.[31] Nevertheless, the resulting
carbon-coated LFP. The resulting layer has a higher graphitic lithium-iron phosphate phase did not exhibit a high capacity
carbon content and fewer oxygen-derived groups, benefiting due to the disorder in the arrangement of lithium and iron,
electron transport.[22] Additionally, an effective approach to with iron occupying the lithium sites.[32] The results showed that
addressing the slow kinetics of LiFePO4 involves integrating it iron prevents lithium from moving through the one-dimen-
with large contact area materials, such as graphene and carbon sional channels in the structure. Hence, it is essential to ensure
nanotubes, to create a large contact area. This approach is that iron and lithium are correctly arranged. The problem was
widely used to develop high-rate hybrid electrodes, aiming to fixed when carbonaceous materials were heated to 700 °C for
minimize the carbon content in the resulting materials.[23,24] the hydrothermal material.[33] During the study in 2003, the
researchers concluded that “hydrothermal synthesis is not a
feasible approach for lithium iron phosphate”,[33] however,
2.1.2. Microwave Heating through subsequent modifications to the synthesis conditions,
Chen et al. identified optimal hydrothermal parameters for
Microwave processing achieves rapid, uniform heating in producing electrochemically active LiFePO4.[34,35] It was deter-
ceramics at lower temperatures than traditional methods. It has mined that a synthesis temperature exceeding 175 °C is
been successfully applied in novel sintering for various necessary to reduce iron disorder and achieve proper lattice
materials.[25] Microwave heating differs from conventional parameters and volume. Additionally, reductants like ascorbic
methods, which heat materials externally internally; instead, acid or sugar prevent the formation of surface ferric films.[36,37]
microwave heating occurs at the molecular level, ensuring a Chen et al. noted hydrothermal synthesis produces well-crystal-
uniform temperature distribution throughout the material.[26] lized material with micron-sized particles, typically a few
Furthermore, this approach demonstrates high repeatability hundred nanometers thick, where the short dimension aligns
and eliminates the requirement for reducing gas. Cost-effective with the diffusion direction Figure 3.[37]
carbon, characterized by fast heat production, is selected as the In 2005, Lee et al. found that LiFePO4 formation in super-
microwave absorbent to ensure effective heat generation. critical water occurred within a narrow pH range under neutral
Carbon can also generate reduced gas, protect ferrous ions and or slightly basic conditions, with pH minimally affecting particle
eliminate iron ions. Figure 2c provides a schematic representa- size or shape.[38] Moreover, they observed that smaller and more
tion of microwave heating.[27] Carbon is a popular microwave uniform particles were obtained in supercritical water synthesis
absorber due to its affordability and rapid heating properties, compared to subcritical water.[39] In addition to batch hydro-
forming a reductive atmosphere to protect Fe(II) and prevent thermal synthesis, the continuous hydrothermal technique was
impurities during LiFePO4 powder production. While carbon is utilized to synthesize pure lithium iron phosphate nano-
the primary microwave absorber, other materials like Fe, particles; see Figure 4 d. Also, the water flow rate significantly
glucose, and yeast cells can improve heat generation efficiency influences particle morphology, and continuous hydrothermal
and influence particle size, Li diffusion coefficient, and capacity synthesis yields smaller and more uniform particles than batch
loss, resulting in larger particle sizes and potential synthesis.[40] Water temperature significantly affects the hydro-
impurities.[28,29] thermal synthesis process for LiFePO4 powders, influencing their
reaction rate, ionization degree, particle size, and crystalline
structure. The structure and electrochemical properties are
2.2. Wet Chemical Processing notably influenced by water flow rate and precursor
concentrations.[41] In addition, various carbon sources, such as
Wet chemical preparation methods, such as hydrothermal/ sugar, ascorbic acid, carbon, multi-walled carbon nanotubes
solvothermal, sol-gel, or co-precipitation techniques, possess a (MWCNTs), and the organic surfactant acetyl trimethyl
distinct advantage over solid-state reactions in achieving ammonium bromide (CTAB), serve as reducing agents during
enhanced homogeneity and thorough mixing of the initial calcination to prevent the oxidation of Fe(II).[42] Hydrothermal
compounds at the molecular level. synthesis conducted with an organic surfactant compound like
CTAB facilitated the production of lithium iron phosphate
powders with high surface areas and enhanced electrochemical
performance.[43] CTAB pyrolysis produced a carbon layer on the

ChemPhysChem 2024, 25, e202400459 (5 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 3. Schematic illustration of hydrothermal synthesis of LFP from iron sulfate.

particle surface, generating a reducing environment that compared to traditional solid-state methods. Precursors like
prevented Fe2 + oxidation. lithium acetate, iron (II) acetate, lithium phosphate, iron (III)
Additionally, hydrothermal synthesis is suitable for prepar- citrate, lithium oxalate, and iron (II) oxalate are commonly used
ing metal-doped lithium iron phosphates.[44] It was revealed in this method. Sol-gel processing enables precise manipulation
that the rotation speed in the reactor significantly affects the of material structure at the nanometer level, starting from the
formation of secondary particles, as evidenced by Figure 4(a–c), early processing stages. Sols consist of colloidal particles
SEM images of samples prepared at various speeds. At 280 rpm, dispersed in a liquid, whereas colloids are solid particles ranging
primary particles take on an elongated spheroidal shape. This from one to a hundred nanometers in diameter. Gels are
non-spherical morphology, consistent at 360 rpm, is attributed interconnected, rigid networks with submicrometer-sized pores
to the olivine structure’s geometry. Conversely, the sample and polymeric chains. Gels encompass various combinations of
prepared at 1150 rpm exhibits a distinct morphology. The substances, classified into four categories: well-ordered lamellar
findings suggest that stirring at 280 rpm is optimal for structures, covalent polymeric networks, polymer networks
producing powder that enhances electrochemical properties.[45] formed through physical aggregation, and particular disordered
LFP obtained from various iron precursors highlights the structures. The precursors are dissolved in appropriate solvents,
substantial impact of precursor selection on the synthesized such as N,N-dimethylformamide,,[48] water with ascorbic acid, or
material’s morphology (Figure 5). Notably, iron oxalate resulted citric acid,,[49–51] as chelating agent, ethylene glycol, and
in hierarchical self-assembled nanoplates, Fe(acac)3 led to the ethanol.[52] Examples of combinations of lithium and iron
formation of thick plates with aggregation and a spindle-like sources include Lithium acetate and iron (II) acetate,[48,49] lithium
morphology, and Fe(gluconate)2 produced microcrystals shaped phosphate and iron citrate with phosphoric acid,[50] lithium
like diamonds.[46] oxalate and iron (II) oxalate, lithium carbonate and iron (II)
oxalate.[51] The sols are converted into gels using standard
procedures, followed by heating at temperatures between 500–
2.2.2. Sol-Gel Method 700 °C in either an inert gas like argon or nitrogen or in a
slightly reductive atmosphere containing 5–10 % hydrogen in
Sol-gel processing of inorganic ceramic and glass materials, argon/nitrogen.[48,52] These temperatures are lower than those
dating back to the mid-1800s, is primarily motivated by its required by the solid-state method, and typically, a one-step
potential for higher purity and homogeneity alongside lower heat treatment is adequate to produce phase pure LiFePO4.
processing temperatures than traditional ceramic powder Besides improving precursor mixing for lower temperature
methods.[47] Sol-gel processing is driven by its potential for synthesis compared to solid-state methods, the sol-gel method
higher purity, homogeneity, and lower processing temperatures offers the advantage of coating evolving LiFePO4 particles with

ChemPhysChem 2024, 25, e202400459 (6 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 4. SEM image (a–c) of LFP synthesized using continuous stirring hydrothermal method at 280, 360, and 1150 rpm speed. Copyright 2014 Elsevier.
Reproduced with permission from reference[45] and (d) LFP synthesized in continuous hydrothermal synthesis at 573 K. Copyright 2007 Elsevier. Reproduced
with permission from.[40]

carbon from solvents or precursor ligands.[51] Composites 2.2.3. Co-Precipitation

containing carbon and iron phosphides can also be produced
using an aqueous sol-gel method with ethylene glycol as a Like sol-gel, the co-precipitation method improves purity,
carbon source and a N2 + 5 vol% H2 calcination atmosphere. crystallization, and particle sizes at lower temps. Homogeneous
Citrate in gel preparation facilitates hierarchical pore formation lithium iron phosphate is synthesized through aqueous co-
in the meso and macro ranges.[50] During high-temperature precipitation of Fe2 + precursor and subsequent heat treatment
treatment under inert or reducing atmospheres, decomposing in nitrogen.[54] Researchers have noticed that raising the temper-
organics coat the LiFePO4 crystals with an amorphous carbon ature of a solution containing Li +, Fe2 +, and P5 + ions above
surface layer. However, the presence of carbon coating reduces 105 °C while adjusting the pH to between 6 and 10 promotes
the density of LiFePO4, thereby decreasing the reversible the formation of LiFePO4 rather than a mixture of Li3PO4 and
capacity of the electrode with an increasing amount of carbon. Fe3(PO4)2. To elevate the solution temperature above that of
The heating rate during calcination significantly influences the pure water, water-miscible boiling point elevation additives
structure of LiFePO4 powders. A slow heating rate tends to such as ethylene glycol, diethylene glycol, or N-methyl
produce a rougher and less porous structure. Conversely, a high formamide are introduced. Once the solution reaches the
heating rate leads to a more porous structure, impacting the solvent’s boiling point, LiFePO4 begins to precipitate. Subse-
electrochemical properties of the powders.[42] In general, several quently, the obtained precipitate is calcined at 500 °C in a
precursors and solvents are used in Sol-gel synthesis to produce slightly reducing atmosphere.[55] The precipitation step in LiFe-
LiFePO4 powders; the solvent used significantly impacts the PO4 synthesis forms the crystalline phase, reducing the required
powder’s structure. Although organic solvents can also be thermal treatment time and temperature compared to ceramic
employed, water is the most often utilized solvent.[53] synthesis.
Additionally, LiFePO4 can be synthesized via aqueous
precipitation of FePO4·H2O followed by carbothermal reduction
of a mixture containing iron (III) phosphate precipitate and

ChemPhysChem 2024, 25, e202400459 (7 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 5. Morphologies of LFP using hydrothermal synthesis prepared from (a,b) Fe(oxalate), (c,d) Fe(acac)3, (e,f) Fe-PMIDA, and (g,h) Fe(gluconate)2. Copyright
2010 Royal Society of Chemistry. Reproduced with permission from reference.[46]

lithium carbonate with carbon as the reducing agent.[56] Nano- significant discharge capacity with excellent retention.[58] LiFe-
crystalline LiFePO4 with enhanced electrochemical performance PO4 nanoplates (< 50 nm thickness) synthesized via coprecipita-
was synthesized through a two-stage process involving lith- tion in ethylene glycol at 180 °C show rapid crystallization
iation of FePO4·xH2O with oxalic acid followed by calcination at within 20 min. Feeding sequence influences crystal growth,
500 °C.[57] LiFePO4/C composite was successfully produced via allowing tuning of orientation and particle size.[59] LiFePO4
sonochemical precipitation and calcination, where Li3PO4 and polycrystalline material synthesized via an eco-friendly co-
FeSO4 in a PVA aqueous solution underwent sonochemical precipitation method shows amorphous structure and stable
treatment, followed by calcination at 600 °C.[58] As a result, both performance up to 800 °C. The material exhibits electronic
calcination and synthesis times were reduced, yielding a suitability with a band gap of 4.1 eV and evolving Li + ions
powder of LiFePO4 particles coated with carbon that exhibited conductivity for potential electronic applications.[60] Moreover,

ChemPhysChem 2024, 25, e202400459 (8 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

coprecipitation can be combined with other techniques to drying represents one such approach. The LiFePO4/C composite
produce LiFePO4 powders with controlled structures and was synthesized using LiH2PO4, FeC6H5O7, and nitrogen-doped
functionalities.[61] Improving the structure and functionality of carbon nanotubes. After mixing the raw materials and N-CNTs
LiFePO4 powders is achieved by incorporating carbon or metal in water, the suspension was frozen with liquid nitrogen and
dopants, effectively addressing challenges such as poor elec- dried in a vacuum freezer. The solidified precursor was heated
tronic conductivity and low Li + diffusion rates. This synergistic in a tubular furnace under a reducing atmosphere to form the
effect results in improved electrochemical reactivity and composite.
enhanced overall performance in Li-ion batteries.[62] Similarly, pristine LiFePO4 and LiFePO4/C composites were
prepared without N-CNTs or with regular CNTs.[70] While solid-
state reaction is commonly used for commercial LiFePO4
2.2.4. Ultrasonic Spray Pyrolysis production, alternative, more cost-effective synthesis methods
are being explored. However, both LiFePO4 and FePO4 phases
Ultrasonic spray pyrolysis generates droplets efficiently, offering exhibit poor electronic conductivity due to singular Fe cation
simplicity, cost-effectiveness, and extensive surface coverage. oxidation states (2 + or 3 +), and limited lithium-ion movement
Despite challenges in small droplet removal, it delivers stable in one-dimensional tunnels hampers achieving high energy
coatings, versatility in precursor solutions, and overall cost- density. Defects and impurities further hinder performance,
effective applications. Moreover, the process is highly effective particularly at high currents.
in swiftly producing fine, clean, and well-crystallized ceramic By offering insights into the optimal approach based on the
particles with controlled size distribution, ensuring high purity, synthesis process and synthesis product, this research is
easy synthesis process control, and precise particle size anticipated to positively affect the LiFePO4 manufacturing
dispersion. Spray pyrolysis holds significance as a technique for sector. Table 1 presents a comparative analysis of many
producing ultrafine powders, providing clear advantages in techniques.
both process control and material quality.[63] The previously
described characteristics make the spray pyrolysis process a
good option in academics to produce LiFePO4 powders to 3. Recycling Processes
improve electrochemical performance.[64–67] The synthesis proc-
ess involves atomizing a precursor solution using an ultrasonic 3.1. General
nebulizer, with the sprayed droplets transported to the reactor
by gas. The reactor temperature varies from 400–600 °C, and The recycling process for LiFePO4 batteries encompasses several
the resulting powders undergo additional sintering at 600– essential steps, including battery collection, disassembly, crush-
800 °C temperatures. Spray pyrolysis with carbon sources can ing, component separation, metal recovery, and the environ-
produce LiFePO4/C powders with lower particle sizes, increasing mentally friendly disposal of non-metallic materials. By follow-
specific surface area. Carbon-coated three-dimensional porous ing these processes, recycling LiFePO4 batteries brings notable
LiFePO4 microspheres are made in a fast processing time (about benefits like decreasing the need for raw materials, preserving
10 min) with improved electrochemical characteristics, consis- energy, and reducing greenhouse gas emissions linked to
tent shape, and 60 μm size by the use of a supercritical and battery production.
spray-dry combination approach.[68] Kashi et al. employed table After collection, the batteries undergo crushing to create
sugar, citric acid, and sucrose as carbon precursors during small fragments, followed by component separation using
ultrasonic spray pyrolysis and calcination to synthesize LFP C magnetic separation, sieving, and chemical processes. The
samples. The addition of sucrose effectively prevents agglomer- recovered metals, like lithium, iron, copper, and aluminum,
ation during calcination, leading to a higher carbon content. undergo further processing to obtain high-purity materials
Electrochemical experiments for Li-ion storage show inferior suitable for reuse. Meanwhile, non-metallic items such as
performance in carbon-free and uncalcined samples. However, plastics, papers, and electrolytes are disposed of properly to
samples containing 2.5 and 5.0 g of sucrose per 100 ml LFP safeguard the environment.
precursor solution demonstrate excellent results.[66] Metal dop- Figure 6 describes the recycling processes for used LiFePO4
ants also ensure high tap density and short production time for batteries. After being retired from an electric vehicle, the used
commercially viable electrode materials. Synthesized LiFeTMPO4 battery undergoes capacity detection and pre-discharging to
nanoparticles by spray pyrolysis, especially LiMn1/3Fe2/3PO4, ensure safety. It is then broken down into separate anode
demonstrate improved electrochemical performance and higher plates, cathode plates, and other parts for treatment. The
practical energy density for cost-effective and high-performance cathode plates are cleaned and dried to produce aluminum foils
battery materials.[69] and LiFePO4 powders. These powders are further processed
through ball-milling and spray drying after being annealed to
remove impurities and tested for element content.[81] Following
2.2.5. Other Methods for Synthesis the initial pretreatment, active materials in spent LiFePO4
batteries are separated using chemical and physical methods
In addition to the mentioned techniques, the quest for like thermal treatment, alkaline leaching, or organic solvent.
innovative and alternative methodologies continues. Freeze- Thermal processes sort materials based on their melting points,

ChemPhysChem 2024, 25, e202400459 (9 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Table 1. A comparative analysis of the LiFePO4 synthesis methods.

Method Materials & Experiment condi- Advantages Results Discharge Ref
concentration tion Capacity
[25]
Microwave - Li2CO3 (99 %) 5–20 min in *Short reaction time *High electrochemical capacity 125 mAh/g
heating - NH4H2PO4 2.45 GHz, with a *Microwave heating and good cycle ability at 10 mA/g
(99 %) power level of is a promising method. * The discharge capacity and 60 °C
- Fe(CH3COO)2 500 W ~125 mAh/g
(95 %)
[19]
Solid-state - α-Fe2O3, - 700 °C for 3 h * Smaller particles size for LiFe- * A better electrochemical per- 138 mAh/g
- LiOH · H2O without PO4 prepared from NH4H2PO4 to formance in the sample pre- at 0.2 C
- NH42HPO4 nitrogen gas flow that prepared from (NH4)2HPO4 pared from NH4H2PO4 and 25 °C
- 5 wt % glu-
cose and
40 wt % oxalic
acid
[20]
Carbothermal - FePO4·4H2O - FePO4 and LiOH * one-step reaction * Discharge capacity of 160 160 mAh/g
reduction - LiOH·H2O ball-milled for 2 h * Suitable for mass production mAh/g at 0.1 C in 30 °C. at 0.1 C
- Polypropy- - 36.8 g of PP per of LiFePO4/C and 30 °C
lene (PP) mole FePO4 at
650 °C for 10 h
[71]
Solid-state re- - LiOH·H2O calcined at 700 °C * Produce particle ranges from * Active ingredient LiFePO4 syn- 154 mAh/g
action - Fe2O3 for 2 h and sintered micrometers to nanometers thesized without carbon coat- at 0.2 C
- H3PO4 at 900 °C for 6 h. * Produce single or multi com- ing and 25 °C
ponent particles * The final phase of LiFePO4 has
* Suitable for industrial applica- a space group Pnma, indicating
tion an olivine structure.
[72]
Carbothermal - FePO4 - Calcined at 350 °C * Controlled morphology for * Spherical particle morphology 164.8 mAh/
reduction - Li2CO3 for 5 h under N2 LiFePO4/C improves tap density and high- g at 0.1 C
- Sucrose atmosphere. * Understanding how small par- rate performance and 25 °C
- Took out the sam- ticles fill voids formed by large * Tap density: 1.3649 g cm 3
ple and ground it. particles, improving tap density and specific capacity of
- Calcined again at * Improved tap density and 94.85 mA h/g at 5 C.
750 °C for 10 h specific capacity
under N2 flow.
[73]
- 15 mmol - 10 h in 180 °C for *Using low temperature *Uniform synthesis of nanorod
Solvothermal LiOH.H2O heat treatment *No other impurities LiFePO4 via solvothermal proc- 167 mAh/g
- 5.5 mmol - 3 h in 550 °C for esses at 0.2 C
H3PO4 carbonization *Good rate and cycle perform- and 25 °C
-5 mmol ance at room temperature
FeSO4.7H2O
- Sucrose for
carbonization
[74]
Hydrothermal - FeSO4·7H2O - Sonication process * Reducing energy consumption * Sonication improved cathode 125 mAh/g
- H3PO4 (85 %) in 30 min * Inexpensive, reducing overall performance. at 0.1 C
- LiOH (98 %) - Heating in auto- production costs * Smaller particles in the raw and 25 °C
- ethylene gly- clave at 180 °C for * Uniform particle size distribu- material mixture led to more
col 24 h. filter, dry. tion, enhancing product quality uniform growth of LFP crystals.
with a molar - Heating at 600 °C
ratio of for 6 h.
3 : 1 : 1 : 1/3.
[75]
Sol-gel Stoichiometric - Dissolved in * Ideal for large-scale produc- * LFP particles obtained range 159 mAh/g
amounts of: ethanol and evapo- tion of LiFePO4 particles with between 50 and 100 nm. at 0.2 C
- LiCH3COO rate at 90 °C for 4 h. high rate retention and capabil- * LFP cells exhibit an initial and 25 °C
- Fe(CH3COO)2 dry. ity. discharge capacity of
- H3PO4 - Calcined at 400 °C * Low calcination temperature, > 150 mAh/g at 50 °C.
- C6H10O4 for 1.5 h. high yield, and excellent cycle * No capacity fading at ambient
- Adipic acid - Calcined again at characterization temperature for up to 100
650–700 °C for cycles.
2.5 h.
[76]
Sol-gel - C6H8O7 - Sonication for 2 h * Use of tissue paper as a * Single-phase of orthorhombic
(1.455 g) in 10 ml H2O. template olivine structured LFP.
- FeC6H5O7 - Add tissue * Sol-gel process for microstruc- * Authenticated formation of 115 mAh/g
(1.106 g) paper and stirred at ture synthesis 1D LiFePO4 microstructures and at 0.1 C
- Li3PO4 60 °C until gel. * Tape-casting process for LiFe- particle clusters.
(161.4 mg), - Gel dried and cal- PO4-MWCNT sheets * Enhanced LiFePO4-MWCNT
- NH4H2PO4 cinates at 600, 700, electrochemistry.
(345 mg) 800 °C.
- Ttissue paper

ChemPhysChem 2024, 25, e202400459 (10 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Table 1. continued
Method Materials & Experiment condi- Advantages Results Discharge Ref
concentration tion Capacity

MWCNT
(100 mg)
[77]
Co-precipita- - Fe(NO3)3 - Co-precipitated * Inexpensive precursors used. * Homogeneous synthesis of 154 mAh/g
tion - LiNO3 powder dispersed * Only water vapor produced, pure olivine LiFePO4. at 0.2 C
- (NH4)2HPO4 in sugar solution, making the process environ- * Excellent stability and 25 °C
- ascorbic acid then dry and heat. mentally friendly * Conductivity of LFP/C compo-
- ammonia - Calcined at 350 °C * LiFePO4 powder well distrib- site increased due to carbon
- Sugar (20 wt for 10 h. uted, avoiding agglomeration scaffold.
% of LFP) - Sintered at 600 °C
for 16 h in nitrogen
flow.
[78]
Co-precipita- - Fe(NO3)3 - Hydrothermal * Innovative High Mixing Con- * Di-hydrous FePO4 with micro- 162 mAh/g
tion (1 M) mixed continuous tinuous Rotating Reactor spherical particles composed of at 0.1 C
- H2O2 (1 M) at 3000 rpm. (HMCRR) Technology. uniform nanoplates with excel- and 25 °C
- (NH4)2HPO4 - Precipitates * LiFePO4/C with mesoporous lent crystallinity.
(1 M) from the outlet to structure, larger specific surface * High-rate capacity with dis-
- Li2CO3 batch reactor at area, and more uniform mor- charge capacity at 10 C reaching
- Citric acid 300 rpm for 3 h. phology composed of nano pri- around 125.4 mAh g 1.
- Anhydrous FePO4, mary particles compared to tra- * Enhanced properties of FePO4
Li2CO3, and citric ditional methods. inherited by LiFePO4/C pre-
acid mixed and cal- pared by HMCRR, showing im-
cined at 650 °C for proved cycling stability and
10 h. outstanding high-rate capacity.
[79]
Ultrasonic - LiH2PO4 - Dissolved in * Convenient home-made spray * Memory effect enhanced from 161 mAh/g
Spray Drying (0.036 mol) 50 mL deionized drying equipment. 1.3 mV–2.9 mV as spray drying at 0.1 C
Method - FeCl2 water and then us- * Spray drying temperature sig- temperature increased.
(0.036 mol) ing ultrasonic nificantly impacted memory ef- * Defect of Li–Fe anti-site
- LiOH atomizer. fect and specific capacity of blocked some [010] channels of
(0.00108 mol) - Tube furnace at electrode materials. LiFePO4 structure, causing re-
- HCl (15 ml 200 °C–350 °C. tardation of Li-ion migration.
37 %) - Spray dried LFP * Specific capacity reduced
- Sucrose powder for 1 h. from 161 mAh/g–151 mAh/g as
(0.85188 g) - Tube furnace at spray temperature increased.
650 °C for 8 h.
[80]
Freeze-drying Stoichiometric - Dissolved in * Effective synthesis process us- * Specific capacity value of 146 mAh/g
amounts 25 mL water and ing freeze-drying method. 164 mAh g 1 obtained at C/40 at 0.1 C
(10 3 mol) of frozen drop-by- * Homogeneous carbon covered rate. and 25 °C
LFP: drop under liquid LiFePO4 sample. * The capacity retention study
- C6H8O7.H2O N2. showed very promising results,
- FeC4H6O4 - Freeze-dried for with more than 97 % retention
- LiOH.H2O 48 h in Telstar Lab after 50 cycles.
- NH4.H2PO4 Freeze-Dryer. * Good reversibility of the mate-
(1 : 1 : 1 : 1) - Calcined twice: rial demonstrated by cyclic vol-
350 °C and 600°. tammetry.
[70]
Freeze-drying Stoichiometric - Dissolved in * Three-dimensional porous * Uniform dispersion of nitro- 159 mAh/g
amounts 20 mL water while LiFePO4 modified with uni- gen-doped carbon nanotubes at 0.1 C
(10 2 mol) of stirring. formly dispersed nitrogen- inside the porous LiFePO4. and 25 °C
LFP: - Instant freezing of doped carbon nanotubes. * Excellent electrochemical per-
- LiH2PO4 the suspension * Superior three-dimensional formance in terms of charge/
- FeC6H5O7 under liquid N2 conductive network enhancing discharge tests, and electro-
- N-doped Car- - drying at 55 °C electronic conductivity and ac- chemical impedance spectro-
bon Nano- in a vacuum freezer celerating lithium-ion diffusion. scopy.
tubes for 48 h.
- Heated in a tubu-
lar furnace at
650 °C under a re-
ducing atmosphere
(H2/Ar, 10/90) for
10 h.

while the chemical method involves dissolving aluminum foil in recovering valuable metals, regenerating and utilizing LiFePO4,
an alkali solution to obtain LiFePO4, collected through filtration. and preparing lithium ferrite.[82]
Recycling of LiFePO4 batteries involves three main approaches:

ChemPhysChem 2024, 25, e202400459 (11 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 6. The recycling and repair processes for spent LFP. Copyright 2019 Elsevier. Reproduced with permission from reference.[81]

3.2. Recycling Strategies of Spent LiFePO4 Batteries 3.2.1. Pyrometallurgy

Pyrometallurgy and hydrometallurgy are commonly employed This approach involves subjecting the material’s metal oxides to
methods for recycling used batteries. Pyrometallurgy involves high temperatures in a furnace to create an alloy using smelting
subjecting used lithium-ion batteries (LIBs) to high temper- and calcination. The pyrometallurgical technique effectively
atures, leading to their physical breakdown. By adjusting the removes the separator, electrolyte, and binder from the battery
molar ratio and subsequently recrystallizing and renewing the through evaporation. The success of the process depends on
constituent parts, valuable metals and components within the various factors such as reaction time, temperature, and the type
spent LIBs can be recovered. On the other hand, the hydro- of purge gas used, which can impact the efficiency of metal
metallurgical process focuses on the recovery of individual recovery and may lead to the emission of hazardous gases. An
metals like lithium (Li), cobalt (Co), manganese (Mn), nickel (Ni), optimal temperature is carefully selected to burn off organic
and iron (Fe) from old LIBs. This process begins by digesting the compounds and polymers without causing undesirable phase
used batteries in an appropriate solvent, such as acid, alkaline, changes. Despite some loss of components, the pyrometallurgy
or natural organic acid, effectively dissolving the metallic process is relatively safe and energy-efficient, thanks to the
elements in the batteries.[83,84] occurrence of exothermic reactions. Furthermore, this method
requires minimal pretreatment and is well-suited for batteries

ChemPhysChem 2024, 25, e202400459 (12 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

that must be sorted appropriately.[85] The widely used techni- recovery of 96 %.[93] A pyrometallurgical recycling process was
ques for treating batteries include smelting, roasting/calcina- tested using two reactor designs for recovering LFP with Al2O3
tion, and pyrolysis. Additionally, there are ongoing studies on and MgO crucibles. In the Al2O3 crucible, lithium recovery was
microwave-assisted carbothermic reduction and salt-assisted 68.4 %, and phosphorus recovery was 64.5 %. In the MgO
roasting. These methods are being explored for their effective- crucible, phosphorus removal was 64 %, and lithium removal
ness in battery recycling and waste management.[86] was 68 %.[94]
Spent batteries are heated to temperatures as high as However, pyrometallurgical processes are not advised due
1400 °C during the smelting process, which is higher than the to their high energy consumption, gas emissions, loss of lithium
melting point of metals and oxides. This leads to the creation of during recycling, and strict requirements for specialist treatment
slag and molten alloys. For example, this method successfully equipment.[95] Hence, pyrometallurgy is not considered effective
recovered cathode materials like LCO, LFP, LMO, and NCM811. for recycling LFP batteries.
Co, Cu, Ni, Fe, and P were efficiently recovered as alloys, while
Li and Mn were transformed into chloride and stored in the
dust using CaCl2. The process achieved high Co, Cu, Ni, Fe, and 3.2.2. Hydrometallurgy
P recovery within 80 min at 1450 °C.[87] In a pyrometallurgical
procedure created by Umicore, the spent LIBs were melted Hydrometallurgy is essential for metal recycling and extraction,
without prior preparation in a shaft furnace. An alloy made of providing a more sustainable and efficient alternative to tradi-
Co, Cu, Ni, and Fe was created as a result of the method. tional pyrometallurgical methods.[96] Hydrometallurgy is used to
However, lithium, manganese, and aluminum were lost in the extract metals from ores or waste materials using liquid
slag without any attempt at recovery. Using chlorination solutions. It involves dissolving metals in a liquid, separating
roasting makes it possible to extract lithium from the slag.[88] and recovering the desired metals from the solution. Compared
The roasting technique is performed at temperatures below to pyrometallurgy, hydrometallurgy has lower energy consump-
the melting point, primarily aiming to reduce metals to a lower tion, reduces greenhouse gas emissions, and allows for the
valence stage. An illustrative roasting technique is carbothermal extraction of specific metals with greater efficiency.[97] These
reduction (CTR), in which reductant carbonaceous materials are techniques can be combined and adapted based on the
mixed with the cathode material and subjected to elevated application, metal recovery goals, and environmental
temperatures, typically ranging from 650–1000 °C.[86] In salt- considerations.[98] Li +, Fe2 + or Fe3 + solutions are acquired by
assisted roasting, the separation of Li and LiFePO4 was done by leaching materials with inorganic and organic acids or oxidation
sodium sulfate-assisted roasting. After roasting, LFP transformed reagents. It is possible to use appropriate acids along with
into iron compounds (Fe2O3 and FePO4) and water-soluble oxidizing agents like H2SO3, NH2OH, and H2O2 during the
LiNaSO4. Soaking the roasted material in water allowed solid- leaching process. Employing supporting agents during leaching
liquid separation, yielding Li3PO4 and FePO4.[89] The principal can achieve more effective recovery of metal ions from spent
outcomes of both smelting and roasting methods encompass LFP materials.[85] There are two forms of leaching utilized for
the production of metal alloys, slag, gases, and precursor metal recovery: nonselective and selective recovery leaching. Li
materials that can be utilized in subsequent hydrometallurgical is recovered from the leaching solution in the selective recovery
processes. approach, and FePO4 is obtained as a leaching residue. In
Pyrolysis is heating metal-containing materials at high contrast, the nonselective strategy recovers the cathode into
temperatures without oxygen, leading to decomposition and the leach solution, including Li, Fe, and PO4.[99]
producing toxic gases. Vacuum pyrolysis, as an alternative
approach, can prevent the release of harmful gases into the
environment, but this technique consumes energy and neces- 3.2.2.1. Inorganic Acid Leaching
sitates expensive equipment.[90] The Umicore process consumes
5000 MJ energy per ton of processed batteries.[88] The cost-effectiveness and wide availability of H2SO4 make it
In the pyrometallurgical treatment of spent LIBs, the typical stand out among mineral acids. It has also performed well in a
recovery rates for Li, Fe, and P can vary based on the specific variety of industrial applications. The selective one-step acidic
process used. For instance, one study reported recovery rates of extraction of lithium (Li) from the Li-Fe P framework can be
approximately 98.93 % for lithium using atmosphere-assisted represented by the following reaction:
roasting.[91] Zhang et al. studied the recycling of LFP batteries
using a sodium salt-assisted roasting method with two different 2LiFePO4 ðsÞ þ H2 SO4 ðaqÞ þ H2 O2 ðaqÞ !
sodium salts: Na2CO3 and NaOH. Na2CO3 was used to break Li2 SO4 ðaqÞ þ 2FePO4 ðsÞ þ 2H2 O ðaqÞ
down LFP, into iron and lithium salts. These were then
separated by magnetic separation, achieving a 99.2 % lithium LiFePO4 and Al in Al-bearing used LFP cathode powder
recovery rate. In the second approach, NaOH oxidized LFP into recycled using H2SO4 leaching. The results demonstrated
different compounds, resulting in a 92.7 % lithium recovery rate leaching efficiencies of 91.53 % for LFP and 15.98 % for Al under
after magnetic separation.[92] Li et al. used NaOH to oxidize Fe ideal conditions. Furthermore, lowering the leaching temper-
(II) in LFP at 150 °C, breaking down its structure and releasing Li ature effectively reduced Al dissolution during the acid leaching
and Fe. Magnetic separation yielded Fe3O4 and a lithium of the used LFP cathode material.[100] During the leaching

ChemPhysChem 2024, 25, e202400459 (13 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

process, oxidizing agents like H2O2, H2SO3, and NH2OH can result Oxalic acid, citric acid, aspartic acid, acetic acid, and formic acid
in more efficient recovery of metal ions from spent LFP are used as leaching reagents instead of inorganic acids. For
materials. For example, by employing stoichiometric H2SO4 and example, Formic acid has been employed as the solvent and
H2O2, Li can be selectively leached into the solution, while Fe H2O2 as an oxidant in a selective leaching process for Li recovery
and P are retained in the leaching residue as FePO4. Under the from LiFePO4 spent.[106] Figure 7b depicts the developed process
optimized conditions, the leaching rate for Li was 96.85 %. The for recovering lithium phosphate from the spent cathode
recovered Li is precipitated as Li3PO4 using Na3PO4, and the powder of LiFePO4 batteries. The resulting product, Li3PO4, with
FePO4 in the leaching residue is directly recovered through a a purity greater than 99 %, was precipitated in situ by directly
burning process.[101] Another study examines an optimized adding a saturated solution of Na3PO4. When oxalic acid leaches
process for recovering LiFePO4 from spent lithium-ion batteries the LFP material, it does not promote Fe2 + oxidation but
using various surfactants (CTAB, SDS, and PEG) on recovered precipitates FeC2O4. Conversely, other potential products such
FePO4.2H2O. This approach achieves 98 % iron and 97 % lithium as Li2C2O4, Li3PO4, and Fe3(PO4)2 demonstrate solubility in acidic
leaching when the mixture is dissolved in 2.5 M sulfuric acid.[102] environments. The proposed reaction can be represented as
Li, Fe, Al, and Cu can be recovered substantially from used follows[85]:
LFP cathode material using the acid-alkaline leaching method,
resulting in a high retrieval rate. The approach involves three 12LiFePO6 þ 6H2 C2 O4 :2H2 O ! 3Li2 C2 O4 þ 3FeC2 O4
fundamental steps: thermal pretreatment, acid leaching, alka- þ 4H3 PO4 þ 3Fe3 ðPO4 Þ2 þ 2LiðPO4 Þ þ 12 H2 O
line leaching, and precipitation. In the first step, the spent LFP
cathode powder is heated at 600 °C for four hours, utilizing an The researchers attained an impressive Li leaching efficiency
H2SO4-based acid to separate Al, Fe, and Cu. In the second step, of 98 % by employing 0.3 M oxalic acid at 80 °C for 60 min, with
the leaching residue undergoes alkaline-based leaching to a solid/liquid ratio of 60 g/L. Using oxalic acid as a leaching
recover Li as LiH2PO4 through chemical precipitation. The entire agent, it can efficiently precipitate approximately 92 % of the
procedure is depicted in the provided Figure 7a.[103] To mitigate iron content as FeC2O4.2H2O from LiFePO4.[107] Another advant-
the detrimental effects of high-concentration H2SO4, researchers age of using oxalic acid as a leaching agent is that it does not
developed a high-temperature activation process to stabilize generate any secondary pollutants, making it environmentally
the LFP olivine structures, followed by low-concentration acid friendly and efficient.[108] An eco-friendly and cost-effective
leaching for metal recovery. This effective method efficiently process was developed using acetic acid as the leaching agent
removes impurities and oxidizes the LFP, resulting in a to selectively recover valuable metals from spent LiFePO4
successful and environmentally friendly battery recycling batteries. With optimized parameters, lithium leaching achieved
process.[104] The process achieves high leaching rates of Li, Fe, an efficiency of over 95.05 % and a selectivity of approximately
and P, with approximately 85.56 % Li and 99.58 % Fe being 94.08 %. The resulting Li2CO3 had a high purity of 99.95 wt %,
successfully recovered as Li3PO4 and FePO4, offering a simple, meeting battery-grade standards. The process is economically
efficient, and industrially feasible approach for battery recycling. viable and incorporates green chemistry principles, offering a
Indeed, besides sulfuric acid, other acids can be used to sustainable solution for recycling spent LiFePO4 batteries.[109]
recycle LiFePO4 batteries. Researchers have explored leaching Generally, lithium may be selectively extracted using
using other acids, such as phosphoric acid (H3PO4). In a organic acids, but large-scale recycling is not practical due to
moderate approach, LFP has dissolved in 0.88 M H3PO4 at their cost. A thorough investigation of risk-free alternatives to
temperatures of 80 °C, followed by filtration to eliminate organic acid leachates is crucial in creating an effective,
undissolved components. Subsequently, the resulting solution financially feasible procedure.
underwent reflux to yield FePO4.2H2O precipitate. After thor-
ough washing with distilled water and ethanol, the residue was
dried at 80 °C, achieving a notable leaching efficiency of Li 3.2.2.3. Oxidation Leaching
recovery of 99 %. Also, nearly all the iron is formed into
FePO4.2H2O residue.[105] Oxidation leaching is a hydrometallurgical process involving
Inorganic acids are preferred in hydrometallurgical proc- oxidizing agents to dissolve metals from ores or materials,
esses for cost-effectiveness and rapid leaching rate in extracting allowing for metal recovery and extraction. For instance, sodium
Li from LFP batteries. However, wastewater management and persulfate (Na2S2O8) can also be used to efficiently oxidize
toxicity concerns must be addressed. Optimization should focus LiFePO4 to FePO4 and cause lithium extraction from the cathode
on minimizing acid concentration, reducing chemical consump- without acid or alkali.[110] It is shown that Na2S2O8 as an oxidant
tion, and enhancing Li product purity and reuse value, can facilitate the recycling of lithium from used LiFePO4
considering the low economic value of LFP cathode material. batteries. This method allows for efficient leaching of over 99 %
lithium from the cathode without the use of acid or alkali. The
process maintains the olivine crystal structure of the raw
3.2.2.2. Organic Acid Leaching material, as shown in Figure 7c, and the resulting Li2CO3
product is of high purity (> 99 %).
Due to the potential risks and environmental impacts associ- In addition to sodium persulfate, another used and effective
ated with using inorganic acids, mild organic acids such as oxidant for handling spent LiFePO4 batteries is H2O2. It acts as a

ChemPhysChem 2024, 25, e202400459 (14 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 7. (a) Recycling process of spent LiFePO4 batteries using alkaline-based leaching method. Copyright 2015 Elsevier. Reproduced with permission from
reference,[103] (b) diagram for recycling spent LiFePO4 batteries using the formic acid-H2O2 leaching system. Copyright 2021 Elsevier. Reproduced with
permission from reference,[106] and (c) schematic illustration of the leaching mechanism that preserves the olivine crystal structure without alteration.
Copyright 2019 American Chemical Society. Reproduced with permission from reference.[110]

ChemPhysChem 2024, 25, e202400459 (15 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

powerful oxidant, breaking down into oxygen and water offering a sustainable solution for selectively reclaiming critical
without introducing any impurities.[111] However, the consider- metals in battery production. Future research should focus on
able costs and expenses associated with treating secondary reducing reaction time, enhancing metal recovery at higher
waste present practical and feasibility challenges when consid- density, and exploring different bacterial strains to minimize
ering the implementation of these methods on an industrial acid consumption and waste treatment challenges.[114]
scale. To address these issues, another study investigates air Although the bioleaching method is energy-efficient and
oxidation-water leaching as a cheap and eco-friendly alternative environmentally friendly, it has not been widely adopted due to
for selectively extracting lithium from the spent LFP cathode problems with long cultivation times, slow process kinetics, low
material. The research achieves high leaching efficiency of solid-to-liquid ratios, and metal toxicity. These issues call for
lithium and effective separation of lithium and iron, showcasing advancements in metabolite production, microorganism metal
a clean and efficient technology for recycling spent LFP tolerance, nutrient cultivation, and process kinetics.[115] Table 2
batteries, aligning with the principles of green chemistry.[112] displays the research findings on different leaching agents,
optimal conditions, and the efficacy of Li leaching.

3.2.2.4. Bioleaching
3.3. Direct Regeneration
Metal extraction from LIBs through bioleaching is an environ-
mentally friendly process. It operates under ambient conditions, Direct regeneration is a non-destructive method for recycling
requiring less energy, resulting in fewer greenhouse gas spent LFP cathodes, restoring their composition and structure
emissions, lower operational costs, and reduced contamination without damage. It substantially cuts recovery costs versus
and processing hazards compared to conventional pyrometal- traditional methods and surpasses other recycling technologies
lurgical and hydrometallurgical methods.[113] Currently, a study in energy efficiency, emissions, and revenues. It demonstrates
successfully used Thiobacillus thioparus bacterium for efficient technical superiority and promises widespread adoption.[124,125]
and eco-friendly leaching of lithium from LFP battery cathodes, Various methods have been documented for the direct
achieving high recovery rates of 65–98 %. The recovered lithium regeneration of depleted LFP cathodes. These methods include
was transformed into Li3PO4 and reused as a culture medium, hydrothermal relithiation, molten salt repair, solid-state sinter-

Table 2. Metal recovery from spent LFP batteries using the hydrometallurgy method.
Leaching Solvent Leaching Condition Resultant (Recov- Resultant (Recov- Efficiency (%) Ref
system ered Li) ered Fe)
Solvent Temp (°C), Time Additive Li Fe
conc. (M) (min)
[102]
Inorganic H2SO4 2.5 60, 240 - Li2CO3 FePO4 97.2 98.5
acid [116]
H2SO4 2.0 70, 120 - Li3PO4 FePO4 97.7 93.3
[101]
H2SO4 0.3 60, 120 H2O2 Li3PO4 FePO4 96.9 0.03
(2.2 vol%)
[117]
H3PO4 0.8 40, 40 H2O2 (4 vol Li3PO4 FePO4 97.6 1.12
%)
[118]
HCl 20 wt % 60, 120 H2O2 (20 wt Li3PO4 FeCl3 92.2 91.7
%)
[107]
Organic Oxalic acid 0.3 80, 60 - Li2C2O4 FeC2O4 98 92
acid [109]
Acetic acid 0.8 50, 60 H2O2 (6 vol Li2CO3 FePO4 95.1 94.1
%)
[106]
Formic acid 1 30, 30 H2O2 (5 vol Li3PO4 FePO4 99.5 0.5
%)
Methyl 4 25, 90 H2O2 (18 %) Li + Fe3 + 94 95 [119]

Sulfonic
[110]
Oxidant Na2S2O8 - 25, 20 - Li2CO3 FePO4 > 99 0.05
[120]
H2O2 2.7 25, 240 - Li2CO3 FePO4 95.4 -
[121]
(NH4)2S2O8 - 40, 60 - Li2SO4 FePO4 99 -
[122]
Fe2(SO4)3, NaCl - 60, 30 H2O2 Li2CO3 FePO4 96.5 0.1
(0.6 mol/g)
[112]
air 600 mL/min 25, 300 - Li2CO3 FePO4 99.3 0.02
[114]
Bioleaching T.thioparus, - 700, 30–60 days - Li3PO4 FePO4 98 -
bacteria
[123]
Lemon Juice 100 % juice 25, 60 H2O2 (6 vol Li2CO3 FePO4 94.8 4.05
%)

ChemPhysChem 2024, 25, e202400459 (16 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

ing, and electrochemical treatment. Hydrothermal relithiation is concentration, and reductant dose during LFP regeneration are
a process used to reinsert lithium ions into spent lithium-ion carefully investigated in this work.[130] Following hydrothermal
battery cathodes. Low-temperature hydrothermal relithiation is regeneration, the particle size distribution (Figure 8b) exhibited
a specific method that achieves this at temperatures at or a narrow and high peak attributed to the dispersion of LFP
below 100 °C, with the help of redox mediators like green particles in the liquid phase.[130]
additives to improve the process efficiency.[126] Xu et al. Molten salt offers superior ionic concentration and diffusion
introduced a clean hydrothermal relithiation process, involving rates compared to aqueous solutions. Li-based eutectic molten
combining low-temperature aqueous solution relithiation with salts serve as both lithium sources and liquid mediums for
rapid post-annealing. Through this method, they successfully reacting with transition metal precursors, facilitating the syn-
demonstrated the direct regeneration to heal the structural thesis of high-performance active materials under ambient
defects of the spent LiFePO4 cathode.[127] A one-step hydro- pressure.[131] Nitrate molten salt systems are suitable for low-
thermal method was employed to regenerate spent LiFePO4 temperature lithium supplementation regeneration with layered
cathode material directly, utilizing Hydrazine as an electron cathode materials such as LCO and NCM. However, this system
donor and reductant, enhancing electrochemical is not appropriate for regenerating LFP because nitrate salts,
performance.[128] A green hydrothermal technique is proposed being highly oxidative, tend to oxidize Fe2 + to Fe3 +.[132] To
for the direct regeneration of spent LiFePO4. The study address this issue, low-temperature lithium nitrate molten salt
investigates the effects of hydrothermal conditions on product along with a carbon reductive environment. By increasing the
performance, finding that controlling these conditions facili- temperature to 300 °C, the melted lithium nitrate ensures close
tates lithium supplementation and enhances electrochemical contact between lithium ions and the surface of spent LFP
performance. Under 200 °C for 3 h (Figure 8a), the regenerated particles, compensating for lost lithium. This approach effec-
LFP shows optimal electrochemical performance, demonstrat- tively capitalizes on the low melting point benefit of nitrate.[133]
ing the potential of this green and efficient method for lithium- Ji et al. used a multifunctional organic lithium salt (3,4-
rich lithium-based products.[129] Yang et al. present a green dihydroxybenzonitrile dilithium) to restore the spent LiFePO4
hydrothermal relithiation technique using Li2SO4 solution as the cathode by direct regeneration.[134] This interaction helps fill
lithium source and Na2SO3 as a reductant to directly regenerate vacancies and creates a reducing environment, preventing the
spent LFP. The impacts of hydrothermal temperature, Li formation of Fe(III) phases. Furthermore, when the salt under-

Figure 8. (a) Regeneration of spent LFP cathode. Copyright 2022 Elsevier. Reproduced with permission from reference,[129] (b) Schematic illustration of the
hydrothermal regeneration mechanism and particle size distribution of spent LFP and regenerated LFP. Copyright 2023 Elsevier. Reproduced with permission
from reference,[130] (c) the process of resynthesizing LiFePO4/C material. Copyright 2019 Elsevier. Reproduced with permission from reference,[137] and (d)
schematic description of Li recovery by electrochemical techniques. Copyright 2023 Elsevier. Reproduced with permission from reference.[140]

ChemPhysChem 2024, 25, e202400459 (17 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

goes pyrolysis, it forms an amorphous conductive carbon layer. have higher research value and significance. As a response,
This layer improves the transfer of lithium ions and electrons, researchers have been exploring innovative approaches for the
thereby enhancing the performance of the cathode. A rapid green recovery and reuse of LFP cathode materials. These
ammonium sulfate (NH4)2SO4 salt is proposed for extracting methods aim to achieve efficient metal reclamation while
lithium and recycling FePO4 from commercial LiFePO4 cathode promoting environmental sustainability and cost-effectiveness.
materials. Compared with the traditional hydrometallurgy This section explores some strategies, highlighting their
recovery process, this method achieves fast delithiation of potential to shape a more eco-friendly and economically viable
LiFePO4 within 5 min at 300 °C and converts LiFePO4 to FePO4 in future for LFP recycling.
an air atmosphere.[135] As for regenerating methods, solid-state Researchers established a novel in-situ recycling process for
sintering stands out as a universal technique and has proven to spent LFP batteries using ultrasound-assisted Fenton reaction
be effective in restoring the capacity of degraded cathodes.[136] and direct cathode material regeneration. In this innovative
For example, a green solid route is introduced to resynthesize approach, an ultrasound-assisted Fenton reaction was utilized
LiFePO4/C materials from spent lithium-ion batteries, to recycle to selectively remove PVDF binders, allowing for the recovery of
valuable resources and reduce environmental pollution.[137] As LiFePO4 cathode materials from current collectors. They effec-
illustrated in Figure 8c, the cathodes were crushed, dried, and tively separated LiFePO4 cathode materials from Al foils with a
heated to remove the binder and separate the cathode powder. high liberation rate. Under optimized conditions, about 97 % of
Subsequent processes involved sintering, mixing with scrap coating materials detached with minimal lithium loss. The
powder containing sucrose and Li2CO3, pressing into tablets, process involved hydroxyl radicals ( OH) degrading PVDF bind-
*

and heating to resynthesize the LiFePO4/C materials with ers, facilitating cathode material separation. The exfoliated
varying Li2CO3 addition amounts.[137] A solid-state method is cathode materials were directly regenerated and reused,
currently reported for regenerating spent LiFePO4, involving exhibiting electrochemical performance comparable to com-
powder homogenization followed by thoroughly mixing a mercial LiFePO4.[141] A straightforward and eco-friendly approach
lithium source and a carbon source via spray drying. Sub- was employed to recycle spent LiFePO4 batteries. The method
sequently, carbon-coated lithium iron phosphate is regenerated involved combining the charging mechanism utilized in LiFePO4
using a high-temperature solid-phase method. The regenerated batteries with a slurry electrolysis process. Researchers could
LiFePO4@C demonstrates restored lattice structure, uniform efficiently separate Li and FePO4 by anionic membrane without
surface carbon coating, and excellent electrochemical requiring additional chemicals. chemicals. In aqueous recharge-
properties.[138] For direct recycling, scrap cathode materials with able LIBs, the charging mechanism of the LFP cathode material
a pristine structure can be regenerated through electrochemical involves oxidizing LFP to FePO4 at a positive potential. During
processes. A proposed relithiation method utilizes a three- this process, Li + ions are released into the aqueous electrolyte
electrode system involving the intercalation of lithium ions into and later recovered. Inspired by this mechanism, researchers
scrapped LFP within an aqueous solution system. This process explored electrochemical Li extraction as a potential method for
employs an H-type electrolytic bath configuration with an recovering Li from LFP cathode materials. Utilizing electro-
anion-exchange membrane, a zinc plate as the anode, scrapped chemical techniques to extract Li ions selectively presents a
LFP suspension as the cathode, and a lithium salt aqueous promising and sustainable route for Li recycling in LIBs.[142]
solution as the electrolyte, ultimately leading to LFP regener- During the slurry electrolysis process, lithium ions are easily
ation through a discharging process.[139] In addition, an electro- extracted and leached from the olivine structure of LiFePO4,
chemical approach is employed for the selective recovery of compensating for the oxidation from Fe2 + to Fe3 + and leaving
lithium from spent LiFePO4 through anodic electrolysis (Fig- FePO4 in the leaching residue (Figure 9a).
ure 8 d). Optimized conditions result in high leaching rates for Mechanochemical technology offers a promising approach
Li (96.31 %), while minimizing leaching of Fe (0.06 %) and P to recycling metals from liquid-liquid-phase LIBs through the
(0.62 %), with an exceptional Li/Fe selectivity exceeding utilization of mechanical forces, such as milling or grinding, to
99.9 %.[140] The main reactions during electrolysis are as follows: initiate chemical reactions that facilitate the separation and
extraction of valuable components from the battery
Anodic reaction : LiFePO4 þ e ! Liþ þ FePO4 electrodes.[143] An economically viable acid-free mechanochem-
ical process has been developed for the selective recycling of
Cathodic reaction : 2Hþ þ 2e ! H2 ðgÞ spent LFP batteries. Researchers selectively extract Li from LFP
cathode materials while preserving FePO4, using sodium citrate
Overall reaction : 2LiFePO4 þ 2Hþ !
as a co-milling agent. The method achieves 98.9 % selectivity
2Li þ þ 2FePO4 þ H2 ðgÞ and is economically viable, offering a promising solution for
efficient and environmentally friendly recycling.[144] Also, a
mechanochemical process was employed by co-grinding spent
LiFePO4 with a cost-effective citric acid agent in a ball mill. After
3.4. New Progress in the Recycling of LiFePO4 grinding, the mixture is dissolved in deionized water and
filtered. By introducing H2O2, lithium extraction reaches an
When discussing metal separation units, eco-friendly and impressive 99.35 %, showcasing highly effective recovery. In
sustainable recovery methods are consistently considered to contrast, iron extraction is much lower at 3.86 %, indicating

ChemPhysChem 2024, 25, e202400459 (18 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 9. (a) Schematic illustration of the leaching mechanism for extraction of Li +. Copyright 2020 Elsevier. Reproduced with permission from reference,[142]
(b) mechanism of the mechanochemical treatment of spent LiFePO4. Copyright 2019 Elsevier. Reproduced with permission from reference,[145] (c) the
simultaneous recovery of valuable metals and iron from mixed types of spent LIBs. Copyright 2019 Royal Society of Chemistry. Reproduced with permission
from reference,[147] and (d) diagram for the rapid regeneration of spent LFP cathode materials. Copyright 2023 Elsevier. Reproduced with permission from
reference.[152]

ChemPhysChem 2024, 25, e202400459 (19 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

selective lithium recovery over iron and using H2O instead of

H2O2 leads to slightly lower extraction efficiencies for both 5. Analyzing the Operational Capacity for
lithium (97.82 %) and iron (95.62 %) under optimal conditions. Recycling LFP Batteries
The reaction proceeds through a minimization-cleavage-recom-
bination process, as illustrated in. Figure 9b. This figure 5.1. Market Share
illustrates how the mechanochemical treatment of spent LiFe-
PO4 results in the effective extraction of metals, demonstrating The global lithium-ion battery market, valued at USD 54.4
the importance of mechanical force and chemical reactions in billion in 2023, is set to undergo robust growth, with a
the recycling process.[145] projected compound annual growth rate of 20.3 % from 2024–
Numerous studies have focused on recycling individual 2030. This surge is primarily driven by the automotive sector,
spent cathode materials, deemed unsuitable for practical with a growing demand for lithium-ion batteries due to their
applications. Recycled mixed cathode materials, including LFP, cost-effectiveness. Researchers highlight the significance of
LMO, LNCM, and LCO, creating a new process is noteworthy. energy storage as essential for human survival, as projections
Zou et al. proposed a recovery process for mixed cathode indicate a demand for 2800 GWh of batteries by 2030 and
materials, such as LCO, LMO, LNCM, and LFP, which involves exceeding 9000 GWh by 2050. As nations shift towards electric
leaching, precipitation, and synthesis steps to obtain purified vehicles, surpassing 50 million globally by 2030, the necessity
materials for cathode synthesis. Analysis results demonstrate for energy storage solutions becomes evident, especially with
nearly 100 % recovery of Ni, Mn, and Co, while approximately replacing traditional fuel vehicles.[153]
80 % of Li is recycled as Li2CO3.[146] A closed-loop process is LIBs serve primarily in consumer electronics, electromobility,
proposed to simultaneously recover various metals from and stationary energy storage. Mobile phones in consumer
complex waste streams of spent LIBs. This study explores electronics rely on LCO (87 %) and NMC batteries (13 %) due to
recycling valuable metals and iron from mixed types of spent their higher energy density than LFP batteries. LFP and LMO
LIBs. It employs selective leaching and solid-phase fabrication batteries excel over LCO in cost and safety, making them
to recover them as new cathode materials, specifically LiFePO4 preferable choices. LFP batteries are widely used in EVs and
and LNMC (Figure 9c).[147] The recycling of mixed spent LIBs electrical storage systems due to their affordability, safety, and
often requires excessive acid consumption and the use of durability. NCM batteries, valued for their high energy density,
multiple redox additives. A salt leaching method was imple- are also standard in EVs, while NCA batteries encounter
mented to address this challenge, utilizing NH4Fe(SO4)2 as a production challenges. In contrast, LMO batteries have limited
redox intermediate for synergistic recovery of valuable metals market share due to their lower energy density and temper-
from mixed spent ternary NCM and LFP batteries. This approach ature performance, allowing LFP and NCM batteries to domi-
achieves high efficiency and selectivity, preserving the environ- nate the market.[154,155] This paper focuses on LIBs utilizing LFP
ment through precipitate recovery and regeneration of new as the cathode active material. With 32,400 tonnes shipped in
materials.[148] A synergistic redox strategy has been introduced 2015, China, the world’s largest producer and consumer of
to recover all elements from mixed systems spent LFP and NCM LiFePO4, held 65 % of the market share worldwide.[156] The
batteries, utilizing thermodynamic calculations to identify self- forecast indicates that the global LFP cathode active materials
promoting reactions. With a less acidic environment, this market will grow significantly from 900,000 tonnes in 2021–
method eliminated the need for additional agents and 9,500,000 tonnes in 2030. This growth is accompanied by an
produced over 100 % leaching rates for manganese, nickel, increasing relative market share, rising from 42 %–51 %. The
cobalt, and lithium.[149] As lithium-ion batteries degrade, their market share of various LIBs is illustrated in Figure 10, with
capacity decreases due to irreversible lithium-ion consumption, forecasts extending up to 2030.
increased internal resistance, and structural damage, reducing
lithium in the cathode and increasing lithium in the anode.
Therefore, a graphite prelithiation strategy can directly reuse 5.2. Collection and Sorting
residual lithium from spent graphite anodes to regenerate
degraded LiFePO4.[150] A graphite prelithiation technique was The public’s understanding of LIB management has grown over
presented to restore wasted LFP and offset Li + ion loss.[151] recent decades as governments enact more battery collection
However, due to the complex pretreatment required in this and disposal regulations, recognizing the need for an extensive
process, there is a need for a faster method to regenerate spent collection infrastructure. Just North America, Asia, and Europe
LFP to save energy and costs. An ultrafast heating method is engage in LIB recycling. The EU has developed various policies
proposed to regenerate spent LFP within seconds, aiming to and strategies to advance battery technologies in alignment
achieve low energy consumption and high efficiency in with decarbonization, energy, raw materials, the circular
regeneration.[152] This method, as illustrated in Figure 9 d, economy, and innovation. With a rising demand for batteries,
demonstrates the temperature variations during ultrafast calci- the EU stresses the importance of boosting production capacity
nation. This process involves exposing the regenerated LiFePO4 and reducing dependency on non-European suppliers, focusing
cathodes to temperatures of 700 °C, 800 °C, and 900 °C for a on achieving climate targets, enhancing industrial competitive-
duration of 20 s each. It visually outlines the key steps of the ness, and ensuring environmental sustainability. This is facili-
high-temperature shock strategy for cathode regeneration. tated through initiatives like the Strategic Action Plan for

ChemPhysChem 2024, 25, e202400459 (20 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 10. LIBs on the global market by chemistries. Copyright CES Online 2024. Reproduced with permission from reference,[157] (paid subscription).

Batteries, which aims to secure raw materials, advance technol- 5.3. Recycling Market
ogy, bolster battery production, cultivate skilled human
resources, and advocate for sustainable battery practices.[158] In The number of batteries available for recycling by 2030 is not
Europe, regulations for battery management are governed by expected to grow at the same rate as the new battery market,
directives such as Directive 2006/66/EC, Directive 2012/19/EU, mainly due to longer battery lifetimes and increased reuse.
and Directive 2000/53/EC, which cover waste batteries, waste While the battery market is predicted to grow annually by
electrical and electronic equipment, and end-of-life vehicles, 27.7 % between 2020 and 2030, the recycling rate is forecasted
respectively. These directives aim to ensure proper collection, to decrease each year. Changes in the recycling rate depend on
recycling, and disposal of various types of batteries, including factors such as battery production scrap volume and the reuse
those used in portable devices, vehicles, and industrial rate, which will be closely monitored and refined in models to
applications. Despite efforts to meet recycling targets, chal- improve accuracy. Additionally, regional dynamics, including
lenges remain in enhancing collection efficiency and reducing battery production and trade, influence the recycling ratio in
landfilling or incineration of spent LIBs.[159–161] different markets. Key indicators for 2022 include monitoring
Meanwhile, federal regulations under the Universal Waste battery production capacity, prices for batteries intended for
Regulations in the USA provide a framework for managing reuse and recycling, and studies on production scrap and
hazardous waste, but LIBs are not considered hazardous and alternative scrap sources to enhance modeling accuracy Circular
are largely excluded. Some states have additional regulations Energy Storage Research forecasts a significant rise in annual
focusing on battery recycling, but there are no defined return flows of LFP batteries, projecting an increase from
recycling targets or penalties for noncompliance. Similarly, in 230,000 tonnes in 2022 to about 900,000 tonnes by 2025, as
China, regulations are being developed to manage waste depicted in Figure 11.[157]
traction batteries, driven by initiatives like the “Energy-saving According to the estimation of Circular Energy Storage, the
and New Energy Vehicles Industry Development Program,” current industrial annual recycling capacity for LFP chemistry is
aiming to establish recycling networks and advanced processes about 200 kilotons, thus falling short of the production waste
for battery reuse.[154,156,158] Collecting batteries, including LIBs, and EoL LFP batteries produced yearly.[157] The situation is
Pb-acid batteries, NiCd batteries, and NiMH batteries, typically expected to change rapidly within a few years: recycling is
involves placing them in designated containers at collection expected to increase almost 10-fold to 1,900 kilotons by 2030,
centers or sorting them directly at treatment plants, often while the amount of recyclables is estimated to be 815 kilotons,
performed manually. Once collected, LIBs are processed of which the actual EoL batteries are 265 kilotons (Figure 12).
collectively as mixed feed, although some industrial facilities The majority of the recycling capacity increase is expected to
may sort them by sub-chemistry, such as LCO, LFP, or LMO. occur in China, where most LFP production is concentrated[163]
However, detailed information about this sorting process is and, thus, where the LFP production waste is born. A list of
often unavailable.[156] current industrial operators recycling LFP chemistry is gathered
in Table 3.

ChemPhysChem 2024, 25, e202400459 (21 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Figure 11. Total amount of LIB waste available for recycling by chemistry. Copyright CES Online 2024. Reproduced with permission from reference,[157] (paid
subscription).

Figure 12. The expected development of LFP recycling capacities vs. recyclables available 2022–2030. Copyright CES Online 2024. Reproduced with permission
from reference,[157] paid subscription).

ChemPhysChem 2024, 25, e202400459 (22 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Table 3. Operational or pilot lithium-ion battery recycling plants having capacity/capability for recycling LFP chemistry. Data retrieved from reference.[157]
Company Region Recycling Recycling Products of the recycling plant Recycling Source
capacity capacity (all the listed products, e. g. not process * Recycling capacity
2023, LFP, 2023, all only products from recycling LFP) phase - Products
tons chemistries, Other information: CES online
tons

Austin Ele- United 26 40 Chemical salts, lithium carbonate, Material re- *- CES online
ments States lithium hydroxide covery https://www.circularenergystor-
age-online.com/therecycling-
market/globalrecyclers/austin-el-
ements/houston
Brunp China 120 000 Aluminum metal, chemical salts, Pre-proc- *-CES online
copper metal, lithium carbonate, essing & https://www.circularenergystor-
precursors, cathode material Material re- age-online.com/therecycling-
covery market/globalrecyclers/brunp/
ningxiang
Argus Media
https://www.argusmedia.com/
en/news/2280302-chinas-brunp-
builds-yichang-battery-material-
complex
CALB China 1000 Aluminum metal, copper metal, Pre-proc- *-CES online
lithium carbonate, precursors essing & https://www.circularenergystor-
Material re- age-online.com/therecycling-
covery market/globalrecyclers/calb/
changzhou
Chizhou Xian China 6 000 (1) Aluminum metal, copper metal, Pre-proc- * Company webpage
New material lithium carbonate, precursors essing & http://www.cnntech.cn/page/
Technology Material re- endchs.html
covery -
CES online: https://www.circular-
energystorage-online.com/
therecyclingmarket/globalrecy-
clers/chizhou-xian-new-material-
technology/chizhou
Full Circle Lith- North 500 Lithium carbonate, Aluminum met- Pre-proc- *- CES online
ium America al, Copper metal essing & https://www.circularenergystor-
Material re- age-online.com/therecycling-
covery market/globalrecyclers/full-
circle-lithium/nahunta
Ganzhou China 60 000 Aluminum metal, copper metal, Pre-proc- *- CES online
Longkai Tech- lithium carbonate, precursors essing & https://www.circularenergystor-
nology Material re- age-online.com/therecycling-
covery market/globalrecyclers/chizhou-
xian-new-material-technology/
chizhou
GEM China 3 000 130 000 Precursors Pre-proc- *-https://cleantechnica.com/
essing & 2021/06/20/gem-is-a-gem-in-
Material re- the-battery-recycling-industry-
covery that-was-inspired-by-a-tooth-
paste-experiment/
& CES online
Guangdong China 12 000 Lithium carbonate, aluminum met- Pre-proc- -*CES online
Weima New al, chemical salts, copper metal essing &
Materials Material re-
covery
Guanghua China 50 000 Cobalt sulfate, nickel sulfate, man- Pre-proc- *CES online
Technology ganese sulfate, iron phosphate, lith- essing & - Company webpage https://
ium iron phosphate, lithium man- Material re- www.ghtech.com/Eapplication/
ganese iron phosphate, lithium covery recovery_100000000297454.
carbonate, and lithium carbonate html
concentrate
Hengchuang China 50 000 Lithium carbonate, aluminum met- Pre-proc- *-CES online
Ruineng Envi- al, chemical salts, copper metal essing &
ronmental Pro- Material re-
tection Tech- covery
nology

ChemPhysChem 2024, 25, e202400459 (23 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

Table 3. continued
Company Region Recycling Recycling Products of the recycling plant Recycling Source
capacity capacity (all the listed products, e. g. not process * Recycling capacity
2023, LFP, 2023, all only products from recycling LFP) phase - Products
tons chemistries, Other information: CES online
tons

Hunan Wu- China 12 000 lithium carbonate, aluminum metal, Pre-proc- *-CES online
chuang Recy- chemical salts, copper metal essing &
cling Technol- Material re-
ogy covery
Jiangxi Gan- China 70 000 anhydrous lithium chloride Battery Pre-proc- * CES online
feng Recycling grade lithium carbonate, lithium essing & - https://www.ganfenglithium.
Technology hydroxide and other products Material re- com/pro3_detail_en/id/164.html
covery
Kyburz Switzerland 300 Lithium iron phosphate, copper, Pre-proc- *CES online
graphite, aluminum, plastics, poly- essing https://www.circularenergystor-
mer foil age-online.com/therecycling-
market/globalrecyclers/kyburz/
freienstein
-https://kyburz-switzerland.ch/
en/battery-recycling
(Lanzhou Jin- China 25 000 Pre-proc-
chuan Re- essing &
source Recy- Material re-
cling Technol- covery
ogy)
Nantong Beix- China 20000 Lithium carbonate, aluminum met- Pre-proc- -*CES online
in New Energy al, chemical salts, copper metal essing &
Technology Material re-
covery
Ningxia Bai- China 15 000 Lithium carbonate, Pre-proc- *CES online
chuan New nickel sulfate, essing & - company webpages
Materials cobalt sulfate, manganese sulfate Material re- http://www.bcchem.com/en/
covery product/100.html

ReElement United 137 Chemical salts, lithium carbonate, Material re- *CES online + https://www.reele-
States lithium hydroxide covery menttech.com/
- https://www.reelementtech.
com/

Roth Interna- Germany 9 000 Copper metal, Aluminum metal, Pre-proc- *- CES online
tional Black mass essing https://www.circularenergystor-
age-online.com/therecycling-
market/globalrecyclers/roth-in-
ternational/wernberg-k%C3 %
B6blitz
Young Poon South Ko- 2 000 Chemical salts, lithium carbonate Pre-proc- *- CES online
rea essing & https://www.circularenergystor-
Material re- age-online.com/therecycling-
covery market/globalrecyclers/young-
poong/seoul
Zhejiang New China 50 000 Lithium carbonate, cobalt chloride, Pre-proc- *CES online
Era Zhong- cobalt sulfate, nickel sulfate, man- essing & - Company webpage http://en.
neng Cycle ganese tetroxide, Material re- zhongnengrecycling.com/prod-
covery uct/

(1): In CES online stated that only LFP accepted and thus the 6000 tonnes capacity to recycle would consist only LFP. In company webpages it is however
stated: “This project can recycle 6000 tons of spent ternary cathode materials annually”.

6. Future Challenges and Perspectives conducted in laboratory settings. Expediting the transition from
experimental stages to large-scale industrial implementation is
Numerous researchers have extensively investigated the recy- imperative. Unlike NCM or LiCoO2 batteries, the recycled
cling of spent LFP batteries. However, current methodologies material from LFP cathodes lacks the value of precious metals.
face significant limitations, and much of the research is Consequently, the intricate and costly recovery process ham-

ChemPhysChem 2024, 25, e202400459 (24 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

pers the industrialization of lithium iron phosphate battery mental and economic impacts, thus facilitating the advance-
recycling efforts. The following briefly describes the challenges ment of more effective recycling initiatives.
encountered in the recycling of spent LFP batteries: 1) LFP
batteries have achieved a substantial market presence within
LIBs, mainly due to the rise of electromobility and stationary Acknowledgements
energy storage. However, the prevalence of LFP in certain
regions poses unique challenges for future recycling programs. This work was supported by the Ministry of Education and
2) Current universal recycling techniques, generally suitable for Culture (Grant agreement number OKM/32/524/2022). EU/
layered oxides, are inadequate for LFP batteries. Mechanical Interreg Aurora/ECOLIB project is acknowledged for financial
processing is being tested on a small scale, while hydro- support.
metallurgical processes are still in the laboratory’s experimental
stage, complicating the recycling process. 3) Compared to
layered oxides, LFP batteries contain fewer metals, which raises Conflict of Interests
questions about the financial viability of their recycling. The
solution is creating a closed-loop system emphasizing the The authors declare no conflict of interest.
importance of refining costs over raw material prices, thereby
making LFP recycling economically feasible. 4) The preliminary Keywords: Lithium iron phosphate · Spent-batteries · LiFePO4
findings from the Life Cycle Assessment cast doubt on the Recycling · Sustainable recovery · LFP market.
presumed environmental advantages of recycling LFP cells. This
underscores the imperative for a thorough examination
encompassing economic and environmental considerations. [1] A. K. Padhi, K. S. Nanjundaswamy, J. B. Goodenough, J Electrochem.
Should profitability prove elusive, policy interventions such as Soc. 1997, 144, 1188–1194.
[2] M. S. Islam, D. J. Driscoll, C. A. J. Fisher, P. R. Slater, Chem. Mater. 2005,
implementing a producer responsibility principle akin to the EU 17, 5085–5092.
model may be warranted. Collaborative endeavors in research [3] A. Nytén, J. O. Thomas, Solid State Ion 2006, 177, 1327–1330.
and development must be undertaken to establish econom- [4] M. Gaberscek, R. Dominko, J. Jamnik, Electrochem. Commun. 2007, 9,
2778–2783.
ically viable and environmentally sustainable practices for [5] S. Franger, C. Benoit, C. Bourbon, F. Le Cras, J. Phys. Chem. Solids 2006,
recycling LFP batteries. Alignment with sustainable resource 67, 1338–1342.
management principles and the capacity to adjust to changing [6] M. S. Song, Y. M. Kang, J. H. Kim, H. S. Kim, D. Y. Kim, H. S. Kwon, J. Y.
Lee, J. Power Sources 2007, 166, 260–265.
recycling issues are prerequisites for this 5) Future research and [7] C. W. Kim, J. S. Park, K. S. Lee, J. Power Sources 2006, 163, 144–150.
development efforts should strongly emphasize creating flexi- [8] M. Gaberscek, R. Dominko, M. Bele, M. Remskar, J. Jamnik, Solid State
ble and scalable procedures specific to LFP batteries. In-depth Ion 2006, 177, 3015–3022.
[9] H. Mahandra, A. Ghahreman, Resour. Conserv. Recycl. 2021, 175,
evaluations of the process’s effects on the environment and 105883.
economy must be performed at every stage. By methodically [10] L. Kavanagh, J. Keohane, G. G. Cabellos, A. Lloyd, J. Cleary, Resources
addressing obstacles, scientists may identify crucial elements 2018, 7, 1–29.
[11] D. Jugović, D. Uskoković, J. Power Sources 2009, 190, 538–544.
impacting expenses and environmental effects, opening the [12] D. Meng, H. Duan, S. Wu, X. Ren, S. Yuan, J. Alloys Compd. 2023, 967,
door for more successful LFP battery recycling programs. 171570.
[13] S. Franger, F. Le Cras, C. Bourbon, H. élène Rouault, J. Power Sources
2003, 252–257.
[14] D. Wang, X. Wu, Z. Wang, L. Chen, J. Power Sources 2005, 140, 125–128.
7. Conclusions [15] M. Koltypin, D. Aurbach, L. Nazar, B. Ellis, J. Power Sources 2007, 174,
1241–1250.
[16] N. J. Yun, H. W. Ha, K. H. Jeong, H. Y. Park, K. Kim, J. Power Sources
Considerable attention has been drawn to LFP as a promising 2006, 160, 1361–1368.
cathode material for lithium-ion batteries, owing to its advan- [17] S. T. Masaya Takahashi, Y. S. Koji Takei, J. Power Sources 2001, 97–98,
tages over conventional materials such as Co and Ni in terms of 508–511.
[18] K. Zaghib, N. Ravet, M. Gauthier, F. Gendron, A. Mauger, J. B. Good-
toxicity and cost-effectiveness. Despite its current commercial enough, C. M. Julien, J. Power Sources 2006, 163, 560–566.
application, there is a pressing need for more economical [19] K. Ding, W. Li, Q. Wang, S. Wei, Z. Guo, J. Nanosci. Nanotechnol. 2012,
production methods. This review explores various synthesis 3812–3820.
[20] C. H. Mi, G. S. Cao, X. B. Zhao, Mater. Lett. 2005, 59, 127–130.
approaches for LFP powders and assesses techniques for [21] X. Zhi, G. Liang, X. Ou, S. Zhang, L. Wang, J. Electrochem. Soc. 2017,
recycling spent LFP batteries, underscoring the importance of 164, A1285–A1290.
recycling and advocating for lithium-ion battery sustainability. [22] H.-C. Chuang, J.-W. Teng, W.-F. Kuan, Colloids Surf. A Physicochem. Eng.
As. 2023, 133110.
While numerous researchers have delved into recycling spent [23] W.-B. Luo, L. Wen, H.-Z. Luo, R.-S. Song, Y.-C. Zhai, C. Liu, F. Li, New
LFP batteries, current methodologies encounter significant Carbon Mater. 2014, 29, 287–294.
limitations, mainly due to experimental constraints in laboratory [24] Y. Li, B. Xing, P. Liang, H. Zhang, K. Zhou, J. Ma, S. Fan, S. Yang, J. Solid
State Electrochem. 2022, 26, 2595–2600.
settings. Challenges, including the absence of precious metals [25] M. Higuchi, K. Katayama, Y. Azuma, M. Yukawa, M. Suhara, in J Power
in recycled LFP cathodes, impede industrialization efforts. Sources 2003, 258–261.
Future research endeavors should prioritize the development of [26] L. Wang, Y. Huang, R. Jiang, D. Jia, Electrochim Acta 2007, 52, 6778–
6783.
adaptable and scalable procedures tailored to LFP batteries, [27] S. Lim, S. Reeve, E. Lekuona, A. Garbayo, T. Le Toux, A. Morse, J. Bowen,
accompanied by comprehensive evaluations of their environ- M. Anand, Adv. Space Res. 2022, 69, 751–760.

ChemPhysChem 2024, 25, e202400459 (25 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

[28] X. F. Guo, H. Zhan, Y. H. Zhou, Solid State Ion 2009, 180, 386–391. [74] E. K. Wagiyo Honggowiranto, Jurnal Sains. Materi. Indonesia 2016, 17,
[29] H. Zou, G. Zhang, P. K. Shen, Mater. Res. Bull. 2010, 45, 149–152. 49–55.
[30] L. Q. Sun, R. H. Cui, A. F. Jalbout, M. J. Li, X. M. Pan, R. S. Wang, H. M. [75] S. B. Lee, I. C. Jang, H. H. Lim, V. Aravindan, H. S. Kim, Y. S. Lee, J. Alloys.
Xie, J. Power Sources 2009, 189, 522–526. Compd. 2010, 491, 668–672.
[31] P. Y. Shoufeng Yang, M. Zavalij, S. Whittingham, Electrochem. Commun. [76] H. Al Shibli, P. Chaturvedi, A. B. Kanagaraj, P. Zaghari, D. S. Choi, J. E.
2001, 3, 505–508. Ryu, J. Compos. Mater. 2024, 58, 435–440.
[32] Y. S. Shoufeng Yang, P. Y. Zavalij, M. Stanley Whittingham, Electrochem. [77] M. R. Yang, W. H. Ke, S. H. Wu, J. Power Sources2005, 539–543.
Commun. 2002, 4, 239–244. [78] T. Zhang, S. Lin, J. Yu, Chem. Eng. J. 2023, 455, 140946.
[33] S. Yang, Y. Song, K. Ngala, P. Y. Zavalij, M. Stanley Whittingham, J. [79] T. Lan, X. Guo, D. Li, Y. Chen, Materials 2021, 14, DOI: 10.3390/
Power Sources2003, 239–246. ma14123193.
[34] J. Chen, M. S. Whittingham, Electrochem. Commun. 2006, 8, 855–858. [80] V. Palomares, A. Goñi, I. G. de Muro, I. de Meatza, M. Bengoechea, O.
[35] J. Chen, S. Wang, M. S. Whittingham, J. Power Sources 2007, 174, 442– Miguel, T. Rojo, J. Power Sources 2007, 171, 879–885.
448. [81] Q. Liang, H. Yue, S. Wang, S. Yang, K. ho Lam, X. Hou, Electrochim. Acta
[36] B. Jin, H. B. Gu, Solid State Ion 2008, 178, 1907–1914. 2020, 330, 135323.
[37] J. Chen, M. J. Vacchio, S. Wang, N. Chernova, P. Y. Zavalij, M. S. [82] N. Fatima, N. Solangi, F. Safdar, J. Kumar, North Am. Acad. Res. 2022, 5,
Whittingham, Solid State Ion 2008, 178, 1676–1693. 76–87.
[38] J. Lee, A. S. Teja, J. Supercrit. Fluids 2005, 35, 83–90. [83] W. Wang, Y. Wu, Resour. Conserv. Recycl. 2017, 127, 233–243.
[39] J. Lee, A. S. Teja, Mater. Lett. 2006, 60, 2105–2109. [84] H. Rostami, J. Valio, P. Suominen, P. Tynjälä, U. Lassi, Chem. Eng. J.
[40] C. Xu, J. Lee, A. S. Teja, J. Supercrit. Fluids 2008, 44, 92–97. 2024, 495, 153471.
[41] F. Ruiz-Jorge, A. Benítez, M. B. García-Jarana, J. Sánchez-Oneto, J. R. [85] D. Saju, J. Ebenezer, N. Chandran, N. Chandrasekaran, Ind Eng Chem
Portela, E. J. Martínez de la Ossa, Nanomaterials (Basel) 2021, 11, 2412. Res 2023, 62, 11768.
[42] T. V. S. L. Satyavani, A. Srinivas Kumar, P. S. V. Subba Rao, Eng. Sci. [86] D. S. Vasconcelos, J. A. S. Tenório, A. B. Botelho Junior, D. C. R. Espinosa,
Technol., Int. J. 2016, 19, 178–188. Metals (Basel)13, pp. 543–5712023.
[43] G. Meligrana, C. Gerbaldi, A. Tuel, S. Bodoardo, N. Penazzi, J. Power [87] G. Qu, J. Yang, H. Wang, Y. Ran, B. Li, Y. Wei, Waste Manage. 2023, 166,
Sources 2006, 160, 516–522. 222–232.
[44] X. Ou, G. Liang, L. Wang, S. Xu, X. Zhao, J. Power Sources 2008, 184, [88] X. Hu, E. Mousa, Y. Tian, G. Ye, J. Power Sources 2021, 483, 228936–
543–547. 228945.
[45] K. Vediappan, A. Guerfi, V. Gariépy, G. P. Demopoulos, P. Hovington, J. [89] L. Zhang, T. Teng, L. Xiao, L. Shen, J. Ran, J. Zheng, Y. Zhu, H. Chen, J.
Trottier, A. Mauger, C. M. Julien, K. Zaghib, J. Power Sources 2014, 266, Clean Prod. 2022, 379, 134748–134757.
99–106. [90] H. Bi, H. Zhu, L. Zu, Y. Gao, S. Gao, J. Peng, H. Li, Waste Manage. Res.
[46] K. Saravanan, P. Balaya, M. V. Reddy, B. V. R. Chowdari, J. J. Vittal, 2021, 39, 146–155.
[91] J. Li, G. Wang, Z. Xu, J. Hazard Mater. 2016, 302, 97–104.
Energy Environ. Sci. 2010, 3, 457–464.
[92] B. Zhang, X. Qu, X. Chen, D. Liu, Z. Zhao, H. Xie, D. Wang, H. Yin, J.
[47] L. Larry, Hench, J. K. West, Chem. Rev 1990, 90, 33–72.
Hazard Mater. 2022, 424, 127586–127595.
[48] N. Iltchev, Y. Chen, S. Okada, J. I. Yamaki, J. Power Sources 2003, 749–
[93] X. Li, F. Zhou, S. Gao, J. Zhao, D. Wang, H. Yin, Waste Manage. 2022,
754.
153, 347–354.
[49] K. F. Hsu, S. Y. Tsay, B. J. Hwang, J. Power Sources 2005, 529–533.
[94] A. Holzer, S. Windisch-Kern, C. Ponak, H. Raupenstrauch, Metals (Basel)
[50] R. Dominko, M. Bele, M. Gaberscek, M. Remskar, D. Hanzel, J. M. Goupil,
2021, 11, 1–22.
S. Pejovnik, J. Jamnik, J. Power Sources 2006, 153, 274–280.
[95] J. J. Roy, B. Cao, S. Madhavi, Chemosphere 2021, 282, 130944.
[51] J. K. Kim, J. W. Choi, G. S. Chauhan, J. H. Ahn, G. C. Hwang, J. B. Choi,
[96] Y. Yang, X. Meng, H. Cao, X. Lin, C. Liu, Y. Sun, Y. Zhang, Z. Sun, Green
H. J. Ahn, Electrochim. Acta 2008, 53, 8258–8264.
Chem. 2018, 20, 3121–3133.
[52] D. Choi, P. N. Kumta, J. Power Sources 2007, 163, 1064–1069.
[97] A. Chagnes, B. Pospiech, J. Chem. Technol. Biotechnol. 2013, 88, 1191–
[53] J. Orlenius, O. Lyckfeldt, K. A. Kasvayee, P. Johander, J. Power Sources
1199.
2012, 213, 119–127.
[98] G. Harper, R. Sommerville, E. Kendrick, L. Driscoll, P. Slater, R. Stolkin, A.
[54] G. Arnold, J. Garche, R. Hemmer, S. Ströbele, C. Vogler, M. Wohlfahrt- Walton, P. Christensen, O. Heidrich, S. Lambert, A. Abbott, K. Ryder, L.
Mehrens, J. Power Sources 2003, 247–251. Gaines, P. Anderson, Nature 2019, 575, 75–86.
[55] Delacourt, THIRUTTU TUOMITTUR US009954227B2 (12) United States [99] J. Kumar, R. R. Neiber, J. Park, R. Ali Soomro, G. W. Greene, S. Ali Mazari,
Patent, 2018. H. Young Seo, J. Hong Lee, M. Shon, D. Wook Chang, K. Yong Cho,
[56] B. Q. Zhu, X. H. Li, Z. X. Wang, H. J. Guo, Mater. Chem. Phys. 2006, 98, Chem. Eng. J. 2022, 431, 133993–133409.
373–376. [100] W. bo Lou, Y. Zhang, Y. Zhang, S. Zheng, P. Sun, X. jian Wang, J.
[57] J. C. Zheng, X. H. Li, Z. X. Wang, H. J. Guo, S. Y. Zhou, J. Power Sources, zhong Li, S. Qiao, Y. Zhang, M. Wenzel, J. J. Weigand, Trans. Nonferrous
Elsevier B. V. 2008, 574–577. Met. Soc. China (English Edition) 2021, 31, 817–831.
[58] D. Jugović, M. Mitrić, N. Cvjetićanin, B. Jančar, S. Mentus, D. Uskoković, [101] H. Li, S. Xing, Y. Liu, F. Li, H. Guo, G. Kuang, ACS Sustain Chem. Eng.
Solid State Ion 2008, 179, 415–419. 2017, 5, 8017–8024.
[59] X. F. Guo, H. Zhan, Y. H. Zhou, Solid State Ion 2009, 180, 386–391. [102] R. Zheng, L. Zhao, W. Wang, Y. Liu, Q. Ma, D. Mu, R. Li, C. Dai, RSC Adv.
[60] M. Sellami, M. Barre, M. Dammak, M. Toumi, Braz. J. Phys. 2021, 51, 2016, 6, 43613–43625.
1521–1528. [103] D. Bian, Y. Sun, S. Li, Y. Tian, Z. Yang, X. Fan, W. Zhang, Electrochim.
[61] C. Gao, J. Zhou, G. Liu, L. Wang, J. Alloys Compd. 2017, 727, 501–513. Acta 2016, 190, 134–140.
[62] D. Mohanty, M. J. Chang, I. M. Hung, Batteries 2023, 9, 515–529. [104] S. Tao, J. Li, L. Wang, L. Hu, H. Zhou, Ionics (Kiel) 2019, 25, 5643–5653.
[63] S. Rahemi Ardekani, A. Sabour Rouh Aghdam, M. Nazari, A. Bayat, E. [105] X. Zhou, W. Yang, X. Liu, J. Tang, F. Su, Z. Li, J. Yang, Y. Ma, Waste
Yazdani, E. Saievar-Iranizad, J. Anal. Appl. Pyrolysis. 2019, 141, 104631. Manage. 2023, 155, 53–64.
[64] M. Konarova, I. Taniguchi, Mater. Res. Bull. 2008, 43, 3305–3317. [106] H. Mahandra, A. Ghahreman, Resour. Conserv. Recycl. 2021, 175,
[65] M. R. Yang, T. H. Teng, S. H. Wu, J. Power Sources 2006, 159, 307–311. 105883.
[66] R. Kashi, M. Khosravi, M. Mollazadeh, Mater. Chem. Phys. 2018, 203, [107] L. Li, J. Lu, L. Zhai, X. Zhang, L. Curtiss, Y. Jin, F. Wu, R. Chen, K. Amine,
319–332. CSEE J. Power Energy Syst 2018, 4, 219–225.
[67] M. R. Yang, T. H. Teng, S. H. Wu, J. Power Sources 2006, 159, 307–311. [108] L. Li, J. Lu, L. Zhai, X. Zhang, L. Curtiss, Y. Jin, F. Wu, R. Chen, K. Amine,
[68] J. K. Kim, CrystEngComm. 2014, 16, 2818–2822. CSEE J. Power Energy Syst 2018, 4, 219–225.
[69] Taylor G. Brandt, Andrew R. Tuokkola, Mengjie Yu, Phil Yong Kim, [109] Y. Yang, X. Meng, H. Cao, X. Lin, C. Liu, Y. Sun, Y. Zhang, Z. Sun, Green
Richard M. Laine, SSRN 2024, 4688784. Chem. 2018, 20, 3121–3133.
[70] X. Tu, Y. Zhou, Y. Song, Appl. Surf. Sci. 2017, 400, 329–338. [110] J. Zhang, J. Hu, Y. Liu, Q. Jing, C. Yang, Y. Chen, C. Wang, ACS Sustain
[71] W. Cheng, L. Wang, Z. Sun, Z. Wang, Q. Zhang, D. Lv, W. Ren, L. Bian, J. Chem. Eng. 2019, 7, 5626–5631.
Xu, A. Chang, Mater. Lett. 2017, 198, 172–175. [111] Y. Yang, X. Meng, H. Cao, X. Lin, C. Liu, Y. Sun, Y. Zhang, Z. Sun, Green
[72] X. Yan, Y. Li, C. Li, H. Wang, T. Wang, Y. Ma, S. Zhang, X. Zhang, W. He, Chem. 2018, 20, 3121–3133.
Solid State Ion 2024, 410, 116535–116547. [112] J. Z. Hao Jin, Q. J. Duoduo Wang, C. W. Yongqiang Chen, Green Chem.
[73] Y. Wang, B. Zhu, Y. Wang, F. Wang, Ceram. Int. 2016, 42, 10297–10303. 2022, 24, 152–162.

ChemPhysChem 2024, 25, e202400459 (26 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH
 14397641, 2024, 24, Downloaded from https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cphc.202400459, Wiley Online Library on [04/06/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
Review
ChemPhysChem doi.org/10.1002/cphc.202400459

[113] A. H. Kaksonen, N. J. Boxall, Y. Gumulya, H. N. Khaleque, C. Morris, T. [141] X. Chen, S. Li, Y. Wang, Y. Jiang, X. Tan, W. Han, S. Wang, Waste
Bohu, K. Y. Cheng, K. M. Usher, A. M. Lakaniemi, Hydrometallurgy 2018, Manage. 2021, 136, 67–75.
180, 7–25. [142] Z. Li, D. F. Liu, J. Xiong, L. He, Z. Zhao, D. Wang, Waste Manage. 2020,
[114] H. Mahandra, G. Hein, F. Faraji, A. Ghahreman, Resour. Conserv. Recycl. 107, 1–8.
2023, 195, 107015. [143] M. Wang, K. Liu, J. Yu, C.-C. Zhang, Z. Zhang, Q. Tan, Cir. Econ. 2022, 1,
[115] J. J. Roy, B. Cao, S. Madhavi, Chemosphere 2021, 282, 130944. 100012.
[116] Y. Song, B. Xie, S. Song, S. Lei, W. Sun, R. Xu, Y. Yang, Green Chem. [144] Q. Zhang, E. Fan, J. Lin, S. Sun, X. Zhang, R. Chen, F. Wu, L. Li, J. Hazard
2021, 23, 3963–3971. Mater. 2023, 443, 130160.
[117] X. Chen, C. Luo, J. Zhang, J. Kong, T. Zhou, ACS Sustain Chem. Eng. [145] L. Li, Y. Bian, X. Zhang, Y. Yao, Q. Xue, E. Fan, F. Wu, R. Chen, Waste
2015, 3, 3104–3113. Manage. 2019, 85, 437–444.
[118] Y. Huang, G. Han, J. Liu, W. Chai, W. Wang, S. Yang, S. Su, J. Power [146] H. Zou, E. Gratz, D. Apelian, Y. Wang, Green Chem. 2013, 15, 1183–
Sources 2016, 325, 555–564. 1191.
[119] P. Yadav, C. J. Jie, S. Tan, M. Srinivasan, J. Hazard Mater. 2020, 399, [147] X. Chen, J. Li, D. Kang, T. Zhou, H. Ma, Green Chem. 2019, 21, 6342–
123068. 6352.
[120] Q. Jing, J. Zhang, Y. Liu, C. Yang, B. Ma, Y. Chen, C. Wang, J. Phys. [148] Y. Hua, Z. Xu, B. Zhao, Z. Zhang, Green Chem. 2022, 24, 3723–3735.
Chem. C 2019, 123, 14207–14215. [149] J. Zou, D. Peng, W. Hu, S. Su, X. Wang, Z. Zhao, S. Wang, D. He, P. Li, J.
[121] H. Shentu, B. Xiang, Y. J. Cheng, T. Dong, J. Gao, Y. Xia, Environ. Zhang, Chem. Commun. 2024, 60, 1778–1781.
Technol. Innov. 2021, 23, 101569. [150] M. Fan, X. Chang, X. H. Meng, C. F. Gu, C. H. Zhang, Q. Meng, L. J. Wan,
[122] Y. Dai, Z. Xu, D. Hua, H. Gu, N. Wang, J. Hazard Mater. 2020, 396, Y. G. Guo, CCS Chem. 2023, 5, 1189–1201.
122707. [151] T. Wang, X. Yu, M. Fan, Q. Meng, Y. Xiao, Y. X. Yin, H. Li, Y. G. Guo,
[123] J. Kumar, X. Shen, B. Li, H. Liu, J. Zhao, Waste Manage. 2020, 113, 32– Chem. Commun. 2019, 56, 245–248.
40. [152] S. H. Zheng, X. T. Wang, Z. Y. Gu, H. Y. Lü, X. Y. Zhang, J. M. Cao, J. Z.
[124] Y. Jin, T. Zhang, M. Zhang, Adv. Energy Mater. 2022, 2201526. Guo, X. T. Deng, Z. T. Wu, R. H. Zeng, X. L. Wu, J. Power Sources 2023,
[125] J. Li, J. Zhang, W. Zhao, D. Lu, G. Ren, Y. Tu, ACS Omega 2022, 7, 587, 233697.
25590–25599. [153] H. Ji, J. Wang, J. Ma, H. M. Cheng, G. Zhou, Chem. Soc. Rev. 2023, 52,
[126] X. Yu, S. Yu, Z. Yang, H. Gao, P. Xu, G. Cai, S. Rose, C. Brooks, P. Liu, Z. 8194–8244.
Chen, Energy Storage Mater. 2022, 51, 54–62. [154] T. Elwert, Q. Hua, K. Schneider, Mater. Sci. Forum, Trans Tech
[127] P. Xu, Q. Dai, H. Gao, H. Liu, M. Zhang, M. Li, Y. Chen, K. An, Y. S. Meng, Publications Ltd 2019, pp. 49–68.
P. Liu, Y. Li, J. S. Spangenberger, L. Gaines, J. Lu, Z. Chen, Joule 2020, 4, [155] E. Fan, L. Li, Z. Wang, J. Lin, Y. Huang, Y. Yao, R. Chen, F. Wu, Chem.
2609–2626. Rev. 2020, 120, 7020–7063.
[128] Q. Jing, J. Zhang, Y. Liu, W. Zhang, Y. Chen, C. Wang, ACS Sustain [156] F. Forte, M. Pietrantonio, S. Pucciarmati, M. Puzone, D. Fontana, Crit.
Chem. Eng. 2020, 8, 17622–17628. Rev. Environ. Sci. Technol. 2021, 51, 2232–2259.
[129] B. Chen, M. Liu, S. Cao, H. Hu, G. Chen, X. Guo, X. Wang, J. Alloys [157] H. Eric Melin, “CES Online Database. Circular Energy Storage Con-
Compd. 2022, 924, 166487. sultants, https://circularenergystorage.com/cesonline.,” 2024.
[130] Y. Yang, Z. Liu, J. Zhang, Y. Chen, C. Wang, J. Alloys Compd. 2023, 947, [158] C. Endo, T. Kaufmann, R. Schmuch, A. Thielmann, benchmarking
international battery policies 2024.
169660.
[159] DIRECTIVE 2000/53/EC OF THE EUROPEAN PARLIAMENT AND OF THE
[131] J. Yang, W. Wang, H. Yang, D. Wang, Green Chem. 2020, 22, 6489–6496.
COUNCIL of 18 September 2000 on End-of Life Vehicles, 2000.
[132] Y. Lan, X. Li, G. Zhou, W. Yao, H. M. Cheng, Y. Tang, Adv. Sci. 2023,
[160] DIRECTIVE 2012/19/EU OF THE EUROPEAN PARLIAMENT AND OF THE
2304425.
COUNCIL of 4 July 2012 on Waste Electrical and Electronic Equipment
[133] X. Liu, M. Wang, L. Deng, Y. J. Cheng, J. Gao, Y. Xia, Ind. Eng. Chem. Res.
(WEEE) (Recast) (Text with EEA Relevance), 2012.
2022, 61, 3831–3839.
[161] DIRECTIVE 2006/66/EC OF THE EUROPEAN PARLIAMENT AND OF THE
[134] G. Ji, J. Wang, Z. Liang, K. Jia, J. Ma, Z. Zhuang, G. Zhou, H. M. Cheng,
COUNCILof 6 September 2006, I, 2006.
Nat. Commun. 2023, 14, 584.
[162] C. O. Database. C. E. S. C. H. Eric Melin, 2024
[135] X. Qu, J. Ma, B. Zhang, J. Zhao, B. Qiu, X. Chen, F. Zhou, X. Li, S. Gao, D.
[163] T. Hettesheimer, C. Neef, I. Rosellón Inclán, S. Link, T. Schmaltz, F.
Wang, H. Yin, J. Clean Prod. 2023, 140428.
Schuckert, A. Stephan, M. Stephan, A. Thielmann, L. Weymann, T.
[136] M. Fan, X. Chang, Q. Meng, L. Wan, Y. Guo, SusMat. 2021, 1, 241–254.
Wicke, Lithium-Ion Battery Roadmap – Industrialization Perspectives
[137] Q. Sun, X. Li, H. Zhang, D. Song, X. Shi, J. Song, C. Li, L. Zhang, J. Alloys
Toward 2030 2023.
Compd. 2020, 818, 153292.
[138] Y. Zou, J. Cao, H. Li, W. Wu, Y. Liang, J. Zhang, Ind. Chem. Mater. 2023,
1, 254–261.
[139] S. Zhou, J. Du, X. Xiong, L. Liu, J. Wang, L. Fu, J. Ye, Y. Chen, Y. Wu, Manuscript received: April 26, 2024
Green Chem. 2022, 24, 6278–6286. Revised manuscript received: September 12, 2024
[140] Z. Qin, X. Li, X. Shen, Y. Cheng, F. Wu, Y. Li, Z. He, Waste Manage. 2024, Accepted manuscript online: September 12, 2024
174, 106–113. Version of record online: November 3, 2024

ChemPhysChem 2024, 25, e202400459 (27 of 27) © 2024 The Authors. ChemPhysChem published by Wiley-VCH GmbH