Journal of Cleaner Production 305 (2021) 127143

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Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Review

A critical review on biochar for enhancing biogas production from

anaerobic digestion of food waste and sludge
Manish Kumar a, b, Shanta Dutta b, Siming You c, Gang Luo d, e, Shicheng Zhang d, e,
Pau Loke Show f, Ankush D. Sawarkar g, Lal Singh a, Daniel C.W. Tsang b, *
a
CSIR- National Environmental and Engineering Research Institute (CSIR-NEERI), Nagpur, 440 020, India
b
Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, China
c
University of Glasgow, James Watt School of Engineering, Glasgow, G12 8QQ, UK
d
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan
University, Shanghai, 200433, China
e
Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China
f
Department of Chemical and Environmental Engineering, Faculty of Science and Engineering, University of Nottingham Malaysia, Jalan Broga, Semenyih,
43500, Selangor Darul Ehsan, Malaysia
g
Department of Computer Science and Engineering, Visvesvaraya National Institute of Technology (VNIT), Nagpur, Maharashtra, 440 010, India

a r t i c l e i n f o a b s t r a c t

Article history: The conversion of food waste and sludge into biogas via anaerobic digestion technology is gaining
Received 1 January 2021 attention in recent years, which plays a significant role in waste valorization into bioenergy and pro-
Received in revised form motes environmental sustainability. Biochar is a carbonaceous material produced via thermochemical
19 March 2021
conversion of biomass waste, and tailoring biochar for diverse environmental applications adheres to the
Accepted 13 April 2021
principle of circular economy. The emerging application of biochar as an additive in the anaerobic
Available online 17 April 2021
digestion of food waste and sludge has been intensively investigated in the last few years. However, a
Handling editor; Kathleen Aviso comprehensive understanding of multifunctional roles of biochar and its mechanisms in the production
of biogas via miscellaneous/complex anaerobic digestion process is yet to be attained. This review
Keywords: scrutinizes the key roles of biochar as an additive and emphasizes the influences of biochar character-
Waste valorization istics on the anaerobic digestion processes and their capability to address the foremost challenges. This
Pyrolysis review also evaluates the techno-economic and environmental impacts of biochar synthesis and its
Black carbon emerging application for biogas production via anaerobic digestion to make the integrated process more
Biomethane production
economical and environmentally sustainable, and identifies challenges and prospects for future studies.
Circular economy
© 2021 Elsevier Ltd. All rights reserved.
Environmental sustainability

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2. Method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3. Tailoring biochar for anaerobic digestion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.1. Synthesis and physicochemical properties of biochar . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.2. Factors influencing biochar characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2.1. Feedstock . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2.2. Temperature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2.3. Heating rate, resident time, and carrier gas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
4. Characteristics of biochar for anaerobic digestion processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
4.1. Porosity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
4.2. Specific surface area . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
4.3. Cation exchange capacity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

* Corresponding author.
E-mail address: [email protected] (D.C.W. Tsang).

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M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

4.4. Electrical conductivity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

4.5. pH . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
4.6. Surface function groups . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
4.7. Redox properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5. Roles and mechanisms of biochar in anaerobic digestion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5.1. Improving the process stability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5.2. Accelerating the process rate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
5.3. Buffering potency and alkalinity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
5.4. Inhibitors adsorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
5.5. Enriched microbial functionality . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
5.6. Electron transfer mechanism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
6. Techno-economic and life cycle analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
6.1. Techno-economic analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
6.2. Life cycle analysis (LCA) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
7. Conclusions and prospects for future research . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
CRediT authorship contribution statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19

Abbreviations HT Human toxicity

HTC Hydrothermal carbonization
AAEMs Alkali and Alkaline Earth Metals HTL Hydrothermal liquefaction
AD Anaerobic digestion IET Interspecies electron transfer
BC_FW Biochar as additives in anaerobic digestion of food IIET Indirect interspecies electron transfer
waste LCA Life-cycle assessment
BC_FW_sludge Biochar as additives in anaerobic digestion of MSS Municipal sewage sludge
food waste and sludge Mt Million tonne
BC_others Biochar as additives in anaerobic digestion of other NH3 Ammonia
waste NHþ 4 Ammonium
BC_sludge Biochar as additives in anaerobic digestion of sludge OCFGs Oxygen-containing functional groups
BET Braunauer-Emmett-Teller OCMSW Organic composition of municipal solid waste
CC Climate change OFMSW Organic fraction of municipal solid waste
CEC Cation exchange capacity OLR Organic loading rate
CH4 Biomethane OM Organic matter
CIC Controlling internal circulation PS Primary sludge
COD Chemical oxygen demand PV Pore volume
D Duration SFGs Surface functional groups
DIET Direct interspecies electron transfer S:I Substrate inoculum ratio
DM Dry matter SS Sewage sludge
EAC Electron accepting capacity SSA Specific surface area
EC Electrical conductivity t Metric tonne
EDC Electron donating capacity T Temperature
EEC Electron exchange capacity TA Terrestrial acidification
EPS Extracellular polymeric substance TAN Total ammonia nitrogen
EU European Union TS Total solids
FAN Free ammonia nitrogen UASB Up-flow anaerobic sludge blanket
FD Fossil depletion USA United States of America
FE Freshwater eutrophication V Volume
FTIR Fourier transform infrared VFAs Volatile fatty acids
FW Food waste VM Volatile matter
GAC Granular activated carbon VOC Volatile organic carbon
GHGs Greenhouse gases WAS Waste activated sludge
GREET Greenhouse gases, Regulated Emissions, and Energy WV Working volume
use in Transportation WWS Wastewater sludge
HR Heating rate WWTPs Wastewater treatment plants
HRT Hydraulic retention time

2
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

1. Introduction waste materials imposing challenges in energy generation and

resource recovery approaches (Elkhalifa et al., 2019; Kapoor et al.,
The worldwide energy crisis, shortage of food reserve, and 2020). At present, a considerable amount of FW and sludge are
generation of hazardous waste are grand challenges distressing the utilized to generate bioenergy/biofuel and valuable products via
socio-economic affairs and impending the environmental sustain- various chemical, thermochemical and biological methods (Wang
ability (Elsayed et al., 2020; Kumar et al., 2020a). Waste generation et al., 2020a; Kumar and Thakur, 2018).
from anthropogenic activities and industrial/agricultural produc- Production of biogas via anaerobic digestion (AD) of organic
tion processes adversely affect the natural environment (Kumar wastes such as primary sludge (PS), waste activated sludge (WAS)
et al., 2020d; Thakur et al., 2018). Food waste (FW) (Xiong et al., (Wei et al., 2020), sewage sludge (SS) with mixed cafeteria FW
2019) and sewage sludge (Kumar et al., 2018; 2016) are two ma- (Wang et al., 2020a), FW alone (Giwa et al., 2019), organic fraction
jor waste streams in municipal solid waste (MSW) disposal, which of MSW (Rasapoor et al., 2020), poultry litter (Indren et al., 2020),
should be appropriately handled to promote a sustainable envi- etc. have been investigated. The produced biogas from AD can be
ronment (Trabold and Babbitt, 2018). FW accounts for approxi- upgraded to biomethane (CH4) and/or used in the generation of
mately 32e62% of the MSW and is anticipated to rise because of heat/energy (Chiappero et al., 2020), and the digestate residue can
rapid urbanization and population growth worldwide (Xu et al., be utilized as fertilizer (Sanchez-Monedero et al., 2018). AD has
2018). The generation of FW is more substantial in high-income been considered as one of the suitable processes for waste bio-
countries, for instance, the European Union (EU) generated 98 valorization built on the syntrophic mechanisms of microbial
million ton (Mt) (Xu et al., 2018), and 63.1 Mt was reported in the communities (Wang et al., 2020a). Hydrolysis, acidogenesis, and
United States of America (USA) (EPA, 2020) (Fig. 1). methanogenesis are three key phases of AD, involving a diverse
The conventional approaches applied for handling and treat- group of microbial communities (Fagbohungbe et al., 2017). Influ-
ment of FW include composting, incineration, and landfilling ential factors include feedstock concentration, inoculum (microbi-
(Zhang et al., 2014a). Landfilling is a conventional approach for FW al) size, process temperature, solution pH, selection of additives,
disposal yet many countries restricted FW landfilling due to limited etc., which can regulate hydrolysis, acidogenesis, and/or meth-
space, emission of greenhouse gases, leachate pollution, etc. anogenesis (Pan et al., 2019; Tang et al., 2020). Hydrolysis of FWs
(Wambugu et al., 2019). For example, the EU has revised the landfill and sludge is a crucial step of the AD, and the rate can be improved
directive to reduce the dumping of organic waste at landfills to 35% by feedstock pre-treatment (Hu et al., 2020a; Fei et al., 2020). Pre-
and below, and Germany bans dumping of all biodegradable waste treatment processes reduce the particle size and improve the
at landfill sites (Cozzolino et al., 2017). Restricting FW landfilling is specific surface area (SSA) of feedstock, facilitate the dissolution of
not only beneficial for the environment but also encourages zero- organic matter (OM) and soluble chemical oxygen demand (SCOD),
waste approach toward sustainable development (Unger and increase biodegradability, and thus improving the CH4 yield (Hu
Razza, 2018). Incineration of FWs is also common yet it is expen- et al., 2020b). Common pre-treatment methods of FW and sludge
sive and energy-intensive, which is not widely feasible, especially include physical and mechanical (Arelli et al., 2020; Fei et al., 2020),
in low-income countries (Zhang et al., 2014a). Considering the high thermal (Li et al., 2017c), chemical (Linyi et al., 2020), and biolog-
water content in FW (70e90%) and the generation of air pollutants ical/enzymatic (Yin et al., 2016) (Table 1). Pre-treatment methods
during incineration, this approach is not sustainable (Wambugu improve the production yield; however, it increases the production
et al., 2019; Nghiem et al., 2017). cost and sometimes is not considered environmentally sustainable
Currently, sludge solids generated in the EU, China, and the USA due to the intensive use of energy and/or chemicals. It has been
are at 10 Mt, 39 Mt, and 7.2 Mt, respectively, and upsurges have recognized that the AD process encounters several challenges such
been predicted with population growth and commercial and in- as low efficiency and stability (Flores, 2020), low organic loading
dustrial expansion (Oladejo et al., 2019; Syed-hassan et al., 2017) rate (OLR) (Hegde and Trabold, 2019), ammonia (NH3) inhibition
(Fig. 1). Considering the projected increase in sludge generation, (Dhar et al., 2016), volatile fatty acids (VFAs) generation (Li et al.,
environmental cost of waste disposal, and stringent environmental 2018), and metal accumulation (Li et al., 2019a), etc.
protocols, novel strategies would be required to advance the sludge To overcome these issues, selected additive carbonaceous ma-
management practices around the world (Ding et al., 2017a; terials have been used for enhancing AD processes (Zhang et al.,
Oladejo et al., 2019). Consequently, utilizing environmental wastes 2018; Kumar et al., 1987). Conductive carbonaceous constituents
as feedstock for fuel and chemical production has recently captured such as granular activated carbon (GAC), carbon cloth (Zhang et al.,
significant attention (Dhote et al., 2020; Morya et al., 2018). 2018) and biochar are preferable materials in view of their capa-
Nevertheless, FW and sludge are considered as heterogeneous bility to facilitate CH4 generation via promoting hydrolysis, acido-
genesis, and methanogenesis, as well as their eco-compatibility
(Tang et al., 2020) (Fig. 2). Biochar offers advantages over other
additives considering their diverse physicochemical characteristics,
governed by feedstock types, synthesis temperature, modification/
activation methods, etc. (Luz et al., 2018a,b; Masebinu et al., 2019).
Recent investigations suggested that biochar possesses specific
characteristics, such as relatively high SSA (Ren et al., 2020),
favourable porosity (Kumar et al., 2020c), abundant oxygen-
containing functional groups (Kumar et al., 2020b), high cation
exchange capacity (CEC) (Luz et al., 2018a,b), and good electrical
conductivity (EC) (Ambaye et al., 2020), etc. (Table 2).
In AD processes, the addition of biochar enhances the removal of
chemical oxygen demand (COD) and reduces the lag phase of
methanogenesis, leading to higher production of CH4 (Wang et al.,
2018a). Besides, the application of biochar in AD enhances the
elemental composition of solid digestate (residue of AD), which can
Fig. 1. Annual generation of FWs and sludge. be further processed and used as fertilizer in the agricultural field
3
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Table 1
Various methods employed for pre-treatment of FWs and sludge in AD operation.

Pre-treatment method Substrate Pre-treatment conditions Highlights of the study Reference

Gamma (g) radiation pre- FW Co-60 g radiation at 8.28-kGy irradiation Improved SCOD up to 70.6%, and 14.3% increments in CH4 was Fei et al.
treatment observed (2020)
Ultrasound pre-treatment FW 480 W/L energy density for 15min SCOD increased by 1.6e1.7 times, improved VFA yield, increased Jiang et al.
reducing sugar and protein contents (2014)
Hydrothermal pre- FW 140  C, 20 min Encouraged dissolution of OM, CH4 yield improved by 31.89% Ding et al.
treatment (2017b)
Thermal pre-treatment FW First at 55 Ce90  C for 70min, then 120 C Improved degradation of Li et al.
e160  C for another 50min VM and VFAS, Improved CH4 yield (2017c)
Microwave pre-treatment Kitchen At 175  C for 1min Improved DOM and CH4 yield by 9% Marin et al.
waste (2010)
Alkaline pre-treatment FW 1% CaO Improved solubilization of OM, achieved biogas yield up to Linyi et al.
1
829 mL g VS and CH4 content 65.48% (2020)
Acidic pre-treatment Kitchen pH ¼ 2 for 24 h SCOD content improved from 32 to 35% Ma et al.
waste (2011)
Thermo-acidic pre- Kitchen Initially at pH ¼ 2 for 24h, SCOD content increased from 32 to 45%, CH4 yield improved by 18% Ma et al.
treatment waste then at 120  C for 30 (2011)
min, then leave at 18  C
Potassium ferrate (K2FeO4) Sludge K2FeO4 ¼ 0.05 g/g TSS Improved SS degradation, Hu et al.
pre-treatment Improved CH4 yield from 8.80 to 11.88 mL g 1VSS d1 (2020a)
1 1
Micro-oxygen pre- Kitchen O2 ¼ 1.11 mL (g VS d ) Improved NH3 degradation, CH4 yield improved by 20.68% Zhen et al.
treatment waste (2020)
Biological pre-treatment FW þ WAS 2 gL-1 fungus inoculums and incubated at Improved sugar content by 85.15%, improved CH4 by 45.58% Yin et al.
100 rpm, 60  C for 24h (2016)

Fig. 2. Biochar as facilitator for promoting the production of CH4.

(Shen et al., 2017). The enhanced contaminant adsorption and producing biogas via AD of FW and sludge in a more economical
abundant surface functional groups of biochar were suggested to be and environmentally sustainable manner. The current review firstly
advantageous in CH4 generation (Ren et al., 2018; Zhang et al., describes the synthesis of biochar, their physicochemical proper-
2020b). The adsorption capacity of biochar mitigated ties, and their roles in the AD of FW and sludge. Various mecha-
contaminants/by-products inhibition, while the surface functional nisms of CH4 production via AD facilitated by biochar addition are
groups may trigger the direct interspecies electron transfer (DIET) deliberated. Finally, techno-economic and life cycle assessment
mechanism among anaerobic microbes (Chiappero et al., 2020; (LCA) aspects are considered for the goal of making the production
Flores, 2020). process more economical and environmentally sustainable. Chal-
The application of biochar as an additive in the AD of FW and lenges and prospects are identified for future research. Further
sludge has been increasingly studied, but there is still a lack of investigations in this domain can encourage a rational design of
critical review related to the roles of specific physicochemical biochar-amended anaerobic digestor with improved stability and
properties of biochar and relevant mechanisms involved in consistency.

4
 Table 2

M. Kumar, S. Dutta, S. You et al.

Synthesis and characterization of biochar for its potential application in AD.

Feedstock Method T ( C) pH D HR SSA PS PV (cm3g1) EC C/N O/C H/C Ash (%) VM (%) Moisture Reference
(%)

Sewage sludge (SS) Hydrothermal 300 6.5 _ _ 57.66 m2g-1 _ _ _ 8 0.19 0.12 _ _ _ Ren et al.
liquefaction (2020)
SS Pyrolysis 350, 550 6.4, 9.5 _ _ _ _ _ 210.7, _ _ _ 41.2, 59.3 _ 0.8, 1.4 Ambaye et al.
442.2 (2020)
mScm1
Corn stover Fast pyrolysis 500 2 _ _ 109.10, 216.08 <1/8 inch _ _ 46.81, 0.270, 0.046, 20.42, 29.27, 6.10, 4.15 Zhou et al.
m2g-1 34.16 0.429 0.040 33.92 28.56 (2020)
Wood pellets Pyrolysis 700, 800 7.41 _ _ _ <50 mm _ _ 6.05 0.144 _ _ _ Zhang et al.
(2020a)
Forest waste Pyrolysis 450, 550, 8.1 _ _ _ _ 133.4, _ 0.125 _ 11.38 _ 11.5 Cimon et al.
273.6 (2020)
mScm1
Corn stover Pyrolysis 600 10.1 _ _ 302.6 m2g-1 <2.3 mm 0.11 25 mScm1 106.36 0.003 0.063 _ _ _ Wei et al.
(2020)
Sludge Pyrolysis 400, 500, 5.61 _ _ 16.99e18.39 19.36e32.23 468.2 _ _ 0.040 0.98e3.20 _ _ Wang et al.
600, 730 e6.13 m2g-1 e635.5 e0.003 (2020b)
mScm1
Algal biomass Pyrolysis 500, 600 _ _ _ 128 m2g-1 12.20 Å 0.15 _ 12.00 _ _ _ 68.41 _ Zhang et al.
(2020b)
Sawdust Pyrolysis 300, 500, _ _ _ _ 0.25e1 mm _ _ _ _ _ _ _ _ Wang et al.
700 (2020c)
 2 -1
WAS Pyrolysis 500 8.01 _ 10 C 41.8 m g _ _ 0.4669 5.49 _ 0.07 66.5 _ _ Yin et al.
min1 dsm1 (2019)
Cow dung and SS Pyrolysis 350e500 6.8 _ _ _ 1e2 mm _ _ 6.54 1.66 0.201 51.58 36.7 8.85 Yue et al.
e11 (2019)
Commercial biochar (CB) and Pyrolysis 500 7.85 20 min _ _ 8.72, 10.5 nm 0.15, 0.11 _ 50.54, 0.098, 0.162, 83.86, _ 4.16, 3.07 Giwa et al.
5

municipal sewage sludge e9.01 5.99 0.001 0.079 52.60 (2019)

(MSS)
Corn straws Pyrolysis 600 7.43 60 min 25 K min1 _ _ _ _ 101.2, 0.083, 0.015, _ _ _ Li et al. (2019a)
100.8 0.131 0.005
Sludge Pyrolysis 300, 500, 6.36 _ _ 12.6e58.1 m2g- 10.7e23.7 nm 0.055e0.307 136.4 _ _ _ _ _ _ Wu et al.
1
700 e7.92 e1174 (2019)
mScm1
Pine Pyrolysis 800 6.29 8h _ 210.78 m2g-1 <5 mm _ _ _ _ _ _ _ _ Lü et al. (2019)
Plant biomass (Ampelodesmos Pyrolysis 450-550, 7 _ _ 121.3e128.7 _ _ _ 20.57 0.88 0.041 19.82 Luz et al.
mauritanicus) m2g-1 (2018)
Sawdust 500 8.01 60min _ _ _ _ _ _ _ _ _ _ _ Li and Feng
(2018)
Sludge Pyrolysis 5.15 _ _ 2890 cm2g1 185.4 mm _ _ 53.3 0.2 0.24 47.4 21.1 1.59 Martínez et al.
(2018)

Journal of Cleaner Production 305 (2021) 127143

Agricultural waste Pyrolysis 700 7.0 3hr _ 397.5 m2g-1 3.921 0.291e0.317 _ 28.09, 0.313, _ _ _ _ Zhuang et al.
e7.5 e4.315 nm 7.58 0.318 (2018)
2 -1
Rice straw Pyrolysis 500 10.58 _ _ 111.5 m g 0.25e0.4 mm _ _ _ _ _ _ _ _ Wang et al.
(2018a)
Sawdust Pyrolysis 500 7.62 1.5 h 10  C 0.25e1 mm _ _ _ _ _ _ 4.65 _ Wang et al.
min1 (2018b)
Vermicompost Pyrolysis 500 8.96 2h 10  C 56.6 m2g-1 5.3 nm 0.075 _ 13.5 0.408 0.076 75.0 ± 0.86 5.3 Wang et al.
min1 (2017a)
Pine sawdust Pyrolysis 650 9.6 _ _ 2 -1
130 m g 3.5e25.9 mm 0.0138 _ 255 _ 0.047 10 Sunyoto et al.
(2017)
Wheat bran pellets, coppiced Fast pyrolysis 800, 500, 7.5 3h _ 55, 61, 13.7 1.7e2 mm 0.0445, 0.048, 49.9, 1.6, _ _ _ _ _ _ Viggi et al.
woodlands, and orchard 500 m2g-1 0.0165 0.5 Sm-1 (2017)
pruning
Rice straw and FeCl3 (1Fe, 10Fe, Carbonization 500 8.53 2h _ _ _ _ _ _ 0.83 _ Qin et al.
100Fe) (2017)
(continued on next page)
 M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

2. Method

Kohlstock et al.

De Vrieze et al.
Sunyoto et al.

Fagbohungbe
Linville et al.

et al. (2016)
0.97, 0.70 Shen et al.

Shen et al.
This review serves to recap the current status, existing tech-
Moisture Reference

Xia et al.

Cai et al.
Meyer-
nologies, and methodological advancement for specific applica-
(2017)

(2017)

(2016)

(2016)

(2016)

(2016)

(2016)

(2015)
tions of biochar in CH4 production via AD using FW and sludge as
feedstock. Peer-reviewed journals, including original research and
2.7, 2.0

reviews, along with important data from commercial applications,

15.2

0.97
were thoroughly reviewed. The literature search was done using
(%)

_
reliable scientific databases, such as Scopus, ScienceDirect,
VM (%)

PubMed, etc., using the keywords CH4 production from FW via AD,

54.10,
95.30
21.2,

45.18,18.69 7.18,

99.0,
12.9

3.73

11.8

7.18
sludge, FW þ sludge (FW_sludge), application of biochar as addi-
_

_
tives in the AD of FW (biochar_FW), biochar as additives in the AD
43.2, 36.3

of sludge (biochar_sludge), biochar as additives in the AD of

Ash (%)

FW þ sludge (biochar_FW_sludge), and biochar as additives in the

45.18
14.3

AD of other wastes (biochar_others) (Fig. 3). This review highlights:

_

_
(1) customization of the physicochemical properties of biochar via
0.004 0.075

0.078

0.047

0.039

0.075
0.06, 0.20,
0.0003 0.09

thermochemical processes; (2) variable properties of biochar that

and
H/C

0.2
_

_
influence the process of the AD; (3) roles of biochar and various
0.087

0.004
mechanisms involved in the production of CH4 via AD of FW and
O/C

0.1

sludge; and (4) techno-economic and environmental impacts of

_

_
207.9

122.4

biochar applications along with challenges and prospects for future

95.6

255
C/N

studies.
_

3. Tailoring biochar for anaerobic digestion

EC

The addition of biochar into the AD process can increase alka-

0.0166, 0.032,
PV (cm3g1)

linity and solution pH, which reduces ammonia inhibition and acid
0.16, 0.11

6.50, 5.07 nm 0.09, 0.23

stress to the microbial community (Xu et al., 2020). Porous nature

0.0120,

0.1180

0.0138

and large SSA of biochar may promote the colonization of bacteria

0.09

and archaea, resulting in an improved AD performance (Martínez

_

et al., 2018; Qin et al., 2017). Abundant surface functional groups

125e177 mm

3.5e25.9 mm
83.27, 39.19,

1.7e2.0 mm

and good EC of biochar can enhance the methane yield via direct or
5, 10 mm
24.45 nm

6.50 nm
0.5 mm

indirect electron transfer mechanism among anaerobic microbes

25.6,

(Chiappero et al., 2020; Baek et al., 2018). The details are discussed
PS

below.
86.5, 792.7 m2g-
51.14, 192.93

315.30 m2g-1
315.2, 353.1
5.48, 16.95,

0.07 m2g-1

2.78 m2g-1
130 m2g-1

3.1. Synthesis and physicochemical properties of biochar

m2g-1

m2g-1
SSA

Synthesis of biochar is generally performed by thermochemical

_

_
1

methods at a temperature range of 300e950  C in reduced oxygen

(O2) environment (Wan et al., 2020b; Wang et al., 2020a). Pyrolysis
(Kumar et al., 2020b; Wang et al., 2020b), gasification (Yang et al.,
HR

2019), and hydrothermal carbonization (Cao et al., 2019; Ruan

_

et al., 2018) are commonly applied for biochar production. Cattle

manure, agricultural residues (Lee et al., 2017; Saffari et al., 2020),
D

10.41, _

forest biomass (Cao et al., 2017), WAS (Yin et al., 2019), anaerobic
8.30,
e9.2

e7.2
9.92

10.3

800e900 8.63

7.86

8.67

digestate (Stefaniuk and Oleszczuk, 2015), algal biomass (Kumar

8.4,
8.6

6.8

9.6
pH

et al., 2020a; Nie et al., 2020), have been utilized as feedstock for
biochar synthesis (Table 2). The thermochemical synthesis
T ( C)

900

450

500

650

650

650

450

600

methods of biochar have been adopted for feedstock with low

moisture content, while HTL is preferred for the feedstock having
moisture contents of more than 70% (w/w) (Cao et al., 2019; Zhao
Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

Pyrolysis

et al., 2016). Pore size, pore volume (PV), SSA, pH, elemental
Method

composition, surface functional groups (CeO, C]O, COOH, OH,

eNHx, etc.), EC, and CEC are key physicochemical properties of
biochar, which affect its environmental applicability and func-
Walnut shell (fine and coarse)

Coconut shell, rice husk and

tionality (Saffari et al., 2020; Wan et al., 2020; Wang et al., 2020a).
The pore structure (micro, meso, and macro) of biochar is related to
its large SSA. Although the SSA of GAC (895 m2 g1) is much larger
Corn stover and pine

than biochar (152 m2 g1), the size of macropores in biochar was

Table 2 (continued )

bigger and wider (1e40 mm) than GAC (1 mm) (Huggins et al., 2016).
Pine sawdust

Corn stover
Fruit waste

The larger microporous size of biochar provides a conducive envi-

Pinewood
Feedstock

Holm oak

wood
Bamboo

ronment for the growth of microbial communities, which would be

better than GAC as an additive in the AD process (Chiappero et al.,
2020). Besides, the pH of biochar is greater than 7 in most cases
6
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

CEC (43.28e321 meq/100 g). These findings establish the potency

of the selected mixture of feedstock and their mixing ratio to
improve the physiochemical characteristics of biochar for different
applications.

3.2.2. Temperature
The biochar synthesized at a lower temperature (300e500  C)
displayed a higher O content (10e40%), and the contents of H, N
reduced at elevated temperature (500e1000  C) (Igalavithana et al.,
2017). For example, Mumme et al. (2014) reported that the pyro-
char produced via pyrolysis at 500  C showed 39.2% w/w ash, 54.7%
w/w dry matter (DM), and pH 9.3, in comparison to hydrochar
produced via hydrothermal carbonization at 230  C, which dis-
played 7.8% w/w ash, 99.8% w/w DM, and pH 4.8. Hydrochar usually
has a lower pH than pyrochar, which is consistent with recent
Fig. 3. Publications in 2010e2020 concerning the production of CH4 via AD process. findings of Ren et al. (2020) and Yin et al. (2019). The thermo-
chemical method and process parameters for biochar synthesis
should be engineered based on feedstock characteristics and cost-
(Table 2), which can neutralize the autogenous acidic environment
effectiveness, with particular attention to the intended
and promote the enrichment of microbial communities
applications.
(Igalavithana et al., 2017; Wei et al., 2020).
Biochar consists of major elements such as carbon (C), hydrogen
3.2.3. Heating rate, resident time, and carrier gas
(H), and oxygen (O), as well as heteroatoms such as nitrogen (N),
Wang et al. (2018a) demonstrate the increase in heating rate
sulphur (S), phosphorous (P), along with metal elements such as
from 2 to 20  C min1 resulting increase in H:C and O:C ratio in
potassium (K), sodium (Na), magnesium (Mg), calcium (Ca), etc.
biochar at 250 and 350  C, thus altering the surface functional
(Kumar et al., 2020c; Liu et al., 2019). The ratios such as H:C, O:C,
groups. Zhang et al. (2009) reported that the elevated HR was not
and N:C determines the amounts and characteristics of O and N
favourable for biochar synthesis, and yield was reduced from
containing surface functional groups present in biochar (Oliveira
22e23% to 8e9% by increasing the heating rate from 5 to 140  C
et al., 2017; Ren et al., 2020). Previous studies (Saffari et al., 2020;
min1. Lee et al. (2017) illustrated the importance of carrier gas in
Chen et al., 2014a) confirmed that the EC of biochar (0.002e23.8
the pyrolysis process and its effect on the physicochemical prop-
dSm1) is generally greater than GAC (3 ± 0.327 dSm1), which
erties of biochar. Biochar synthesized in the presence of CO2
plays a key role in the emerging utilization of biochar as an additive
showed a higher SSA (109.15 m2 g1) than that of N2 (32.46 m2 g1);
in the AD process. Overall, these tunable physicochemical charac-
nevertheless, the presence of CO2 decreased the yield of biochar
teristics of biochar make it a promising material as catalyst support,
because the dual nature of CO2 as a facilitator can accelerate the
adsorbent, microbial habitats, pH buffer, and electron carrier for
breakdown of VOCs and as a reactant can react with feedstock.
enhancing the efficiency of the AD process (Oliveira et al., 2017;
Specific interactions may occur subjected to various parameters
Ponnusamy et al., 2020; Qiu et al., 2019). An inclusive assessment of
such as temperature, heating rate, duration, carrier gases, etc.,
the above-mentioned biochar characteristics and their subsequent
during the synthesis of biochar (Wang et al., 2018a), which require
interactions with the desirable microbial communities should be
extensive understanding for customizing application-oriented
further considered in future studies.
biochar for the AD process.

3.2. Factors influencing biochar characteristics 4. Characteristics of biochar for anaerobic digestion
processes
Several studies suggested that the physicochemical characteris-
tics of biochar are highly governed by its feedstock types, synthesis Based on the engineered synthesis conditions, the characteris-
methods, and associated process parameters (e.g., temperature, tics of biochar can be improved for the sake of its specific appli-
heating rate, residence time, and carrier gas) (Table 2). To design the cation. Biochar properties such as porosity, SAA, CEC, EC, redox
desirable properties of biochar for specific purposes, it is essential to properties, pH, and surface functional groups play vital roles in the
fully understand the physiochemical characteristics of biochar and AD process (Chiappero et al., 2020; Flores, 2020; Qiu et al., 2019),
their influence on the AD process as discussed below. which are discussed in detail below.

3.2.1. Feedstock 4.1. Porosity

The characteristics of biochar are closely associated with feed-
stock compositions (El-Naggar et al., 2018; Wang et al., 2020a). Liu The biochar porosity is considered as a key factor to recognize
et al. (2019) reported that hydrochar synthesized from cow manure the plausible relations with microbes involved in AD. The pore size
feedstock displayed lower C content and higher N content than of biochar can provide microhabitats to aerobic and anaerobic
corn stalk. Pan et al. (2019) reported that higher lignin and fixed C microbes to proliferate (Luz et al., 2018a,b). The representative sizes
content in feedstock led to the synthesis of biochar, having of the microbes involved in AD are bacteria/archaea (0.3e13 mm),
improved SSA and higher surface functional groups. Similarly, fungus (2e80 mm), and protozoa (7e30 mm) (Luz et al., 2018a,b).
biochar derived from rice husk, coconut, and wood displayed Besides, porous biochar facilitates biofilm formation, which acts as
43.28 ± 1.49 meq/100 g, 31.17 ± 0.35 meq/100 g, 21.47 ± 0.65 meq/ a shield for the selective enrichment efficient microorganisms
100 g CEC, respectively (Fagbohungbe et al., 2016). Oh and Seo meticulously involved in the AD process under acid stress condi-
(2016) used mixed feedstock (plastic polymers and rice straw) to tions (Luo et al., 2015). Several bacterial sp. were selectively
synthesize biochar at 550  C with improvement in SSA enriched in the anaerobic digesters augmented with biochar.
(16.4e27.5 m2 g1), pH (9.12e11.4), C content (55.8e58.1% w/w), Amongst archaea, most investigations recognized methanolinea,
7
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

methanosaeta, methanobacterium, and methanosarcina sp. in 4.4. Electrical conductivity

biochar-augmented anaerobic digester. Various investigations
described the spatial dispersal of archaea and bacteria by segre- The syntrophic activities conducted by microbes largely depend
gating the sludge samples into several fractions (Luo et al., 2015; upon the EC (Luz et al., 2018a,b). However, biochar EC was found
Zhao et al., 2016). Lü et al. (2016) hypothesized the methanogens’ not significant compared to the digestate EC, which depends on the
spatial distribution in the pores of biochar by their distinct composition and metabolism of microbial strains (Martins et al.,
morphology and size. The larger leathery appearance of Meth- 2018). Biochar’s capability to promote DIET is equivalent to GAC,
anobacterium (1.2e120 mm) was restricted to biochar pores, despite the notably lower EC of biochar (Chen et al., 2014b; Park
whereas the small, leathery appearance of Methanosaeta et al., 2018). Barua and Dhar (2017) reported that owing to DIET, a
(0.8e7 mm) was distributed across external and internal pores of high EC of 0.2e36.7 mS cm1 was observed in multiple microbial
biochar (Lü et al., 2016; Whitman et al., 2006). These diversely species collected from AD. Martins et al. (2018) suggested that
distributed, enriched microbial communities in biochar pores could conductive substances such as humic substances could behave as
enhance the production of CH4 during the process of AD (Luz et al., electron transporters by donating and receiving electrons to
2018a,b). accelerate DIET.
Wang et al. (2019) evaluated the significance of EC of biochar
synthesized from sawdust and SS in syntrophic oxidation of VFAs.
4.2. Specific surface area
Sawdust biochar was found to promote microbial activities and
VFAs degradation via DIET, owing to the existence of redox-active
The SSA of biochar is considered one of the key factors along
structures. However, no such productivity in AD was observed
with others in the adsorption of environmental contaminants (Luz
due to the addition of SS biochar, although the EC values of sawdust
et al., 2018a,b). Sethupathi et al. (2017) measured the capacity of
biochar and SS biochar were similar. Batch experiments were per-
biochar to remove CO2, H2S etc., in a designed biogas fermenter
formed in the presence of propionate or butyrate under
using four types of biochar. The removal capacity of biochar for CO2
methanogenesis-inhibited conditions, which confirmed the bio-
and H2S was 0.208 mmol g1 and 0.126 mmol g1, respectively. In
char’s electron-accepting capacity (EAC) in the syntrophic process
an investigation on CO2 adsorption by biochars obtained from
and enhancement in acetate production. A control reactor with a
hickory wood and bagasse, Creamer et al. (2014) realized that it was
non-conductive material (i.e., negligible effect on propionate and
effectively achieved due to the physical adsorption through a high
butyrate) demonstrated the significance of biochar’s physical
SSA and N2 groups. The role of biochar pore size (0.5e0.8 nm) (Fiore
properties and its electrical properties in the generation of CH4 via
et al., 2018) and high SSA (Hao et al., 2013) were highlighted for CO2
AD process (Martins et al., 2018). Viggi et al. (2017) evaluated the
sequestration, while the presence of alkali and alkaline earth
AD of FW with two separate controls, one with silica sand and the
metals and basic surface functional groups also played important
other without biochar, where the latter showed more efficient
roles (Chen et al., 2014b).
production of CH4 and VFAs degradation, illustrating the impact of
electrical properties of biochar.
4.3. Cation exchange capacity
4.5. pH
When the concentration of ammonium (NHþ 4 ) and NH3 are
maintained under an optimized threshold for an AD system, it can The biochar conductivity and its microbial association in AD are
aid to provide buffer capacity for balanced bacterial growth, while highly influenced by the pH (Yin et al., 2019). The biochar pH values
the surplus amount of total NH3/freeNH3-N (TAN/FAN) can lead to generally fall within the alkaline range due to ash content and
AD failure (Rajagopal et al., 2013; Zhang et al., 2011). It was docu- volatilization of acidic functional groups, and biochar pH often in-
mented that TAN concentration between 1.7 and 14 g L1 reduced creases with the increase in the pyrolysis temperature (Ren et al.,
the CH4 production by 50%, Methanogens were the most hampered 2020; Yin et al., 2019). Besides, biochar can accept or donate elec-
by an increased FAN concentration (Ho and Ho, 2012; Rajagopal trons due to its inherent redox properties (Yuan et al., 2017) and the
et al., 2013). FAN exerted a negative effect on anaerobes between presence of poly-condensed aromatics, quinones and phenolic
150 and 1200 mg L1 (Poirier et al., 2017; Yenigün and Demirel, groups as electron-accepting and donating species (Klüpfel et al.,
2013). It has been observed that biochar could efficiently alleviate 2014; Yuan et al., 2017). Biochar was found to elevate the alka-
NH3 inhibition, enhancing CH4 production by reducing the lag linity (minimum pH  6) of AD, promoting better microbial action
phase in the reactors due to its strong CEC. Mumme et al. (2014) for quick CH4 production and adaptability to initial loading shock
observed that biochar derived from wheat husk and sludge could (Li et al., 2017a). According to Lü et al. (2016), under an acidic
restrict benign NH3 inhibition at 2.1 g TAN kg1. Shen et al. (2017) (pH ¼ 5.3) stressed situation, biochar could effectively facilitate
promoted the beneficial use of biochar in SS AD, and Su et al. methanogenesis phase, which could improve the operating ca-
(2019) asserted that the NH3eN up to 1500 mg L1 could be alle- pacity with higher organic loadings and increased total solids (Ren
viated by biochar addition in FW AD (Ciccoli et al., 2018). Similarly, et al., 2020). Therefore, with the addition of biochar, a continuous
Lü et al. (2016) reported that high NH₄⁺ stress (up to 7 g-N L1) in an AD system can work with shorter hydraulic retention time (HRT)
AD could be overcome by biochar addition. The involved mecha- and handle the extra OLR.
nisms were believed to include: physical and/or chemical adsorp- Linville et al. (2017) investigated the effects of walnut shell-
tion capacity, surface functional groups (Shen et al, 2016, 2017), CEC derived biochar on the thermophilic and mesophilic setting in the
(Shen et al, 2015, 2017), microbe immobilization (Lü et al., 2016; Su AD of FW, where biochar could enhance the stability by improving
et al., 2019) and advancement of DIET (Lü et al, 2016, 2018). the alkalinity to 4800e6800 mg L1 from 2800 mg L1 CaCO3
Therefore, depending on the operating conditions of AD (e.g., (pH > 8). In a similar study by Wei et al. (2020), corn stover-derived
temperature and pH), substrate, and biochar, it may achieve NH3 biochar (erich in alkaline earth metals) amended reactor showed
mitigation by indirect pathways (via microbe immobilization and effective solids elimination and high CH4 production in a primary
DIET) and/or direct adsorption effects (depending on surface sludge AD. The enhanced buffering capacity of the reactor was
functionality, CEC, etc.) (Flores, 2020; Luz et al., 2018a,b; Tang et al., attributed to the alkalinity increase to 3500e4700 mg L1 CaCO3 by
2020). biochar addition. According to Ambaye et al. (2020), SS biochar
8
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

amended reactor facilitated the fruit waste AD by elevating VFAs than the soluble fraction of biochar alone. The study of Kappler et al.
degradation and CH4 production. Attention should be paid to (2014) also investigated the role of biochar as an electron shuttler
maintain biochar acid-buffering capability and contents of trace between bacteria and Fe(III). There are relatively few studies
elements, such as ash content and alkali and alkaline earth metals proving the mechanisms involved in the biochar redox-facilitated
(AAEMs). It is imperative to optimize the amount of biochar needed AD process, in which a knowledge gap still exists and requires
for all these functions as a higher dose can be detrimental to the more mechanistic studies in the future.
whole AD setting (Linville et al., 2017; Wei et al., 2020).
5. Roles and mechanisms of biochar in anaerobic digestion
4.6. Surface function groups
Biochar inherent properties can encourage microbial biofilm
The composition of biochar surface includes variable functional formation (improves methanogens colonization) and adsorb in-
groups such as eOH, CeO, eCOOH, C]O, eNHx, etc., which aid its hibitors such as NH3 and acetate (Masebinu et al., 2019) (Fig. 4). In
multiple functionalities, including nutrient retention and contam- the AD process, biochar is also used to develop a microbial pro-
inant removal (Kumar et al., 2020b, 2020c). Biochar showed tective layer that stimulates CH4 production. Biochar also serves as
promising results in the NH3 adsorption from digestate and a stabilizing agent by controlling the nutrient access to bacteria and
wastewater. The presence of porous structure and relatively high removes VFAs and NH3 upon its addition to the high solids diges-
SSA is helpful in the physical sorption (Yin et al., 2017), although tate (Indren et al., 2020). The latest literature regarding the roles of
they were not considered as the prominent parameters in NH₄⁺ biochar for enhancing the AD of FW and sludge are summarized in
adsorption in some studies (Kizito et al., 2015; Takaya et al., 2016). Table 3.
For example, ion exchange can also take place between NH₄⁺ and
acidic functional groups on the biochar surface (Wang et al., 2015; 5.1. Improving the process stability
Yin et al., 2017), and CEC can play a role in elevating the biochar’s
NH₄⁺ adsorption capacity (Zeng et al., 2013; Zhang et al., 2014b)In a To ensure an uninterrupted biowaste conversion, the stability of
study by Sahota et al. (2018), biochar was employed for the H2S the AD is essential, which can be improved by the use of biochar via
removal from biogas and achieved 84.2% removal efficiency. Simi- NH3eN alleviation (Lü et al., 2016). Under acid and NH3 inhibition,
larly, Kanjanarong et al. (2017) achieved 98% H2S removal efficiency biochar can enrich the methanogenic microbes, which eventually
(8.02 mmol g1) using biochar and indicated that OH radical and support the degradation of N2 rich substrates and decrease NH3
COOH groups were found accountable for H2S adsorption. Unlike inhibition, resulting in an improved AD performance (Indren et al.,
physical adsorption, H2S adsorption involves chemical reactions 2020). Shen et al. (2016) observed that biochar addition could
with surface functional groups of biochar (Bamdad et al., 2018). reduce the prime inhibitor of AD (free NH3) by up to 10.5% and
promote methanogenesis under acidic stress. Biochar could effi-
4.7. Redox properties ciently raise the alkalinity (pH  6) of the AD, thus assisting the
microbial adaptation to initial loading shock and elevate their ac-
The redox properties of biochar have been considered as a key tivity under organic loading for greater CH4 generation (Li and Feng,
parameter in the AD process (Wang et al., 2019), as well as bio- 2018; Li et al., 2017b).
hydrogen production and energy storage/conversion device However, some adverse effects were associated with the
(Kumar et al., 2020b,c). The redox properties of biochar are gov- excessive biochar input (4.4e4.97 g biochar per gram of dry
erned by its surface functional groups, presence of free radicals, and sludge), such as reduced microbial kinetics and activity inhibition
metals and metal oxides (Chaco
n et al., 2020). For instance, (Shen et al., 2016). Thus, the biochar dosage needs prior optimi-
phenolic CeOH fractions have been recognized as the key func- zation and continuous monitoring to curtail the negative impacts
tional groups accountable for their electron-donating capacity on microbial metabolism and the generation of intermediates
(EDC), whereas quinoid C]O fractions for its EAC (Klüpfel et al., metabolites.
2014). Collectively, they govern the electron exchange capacity
(EEC) (EEC ¼ EDC þ EAC) of the biochar. The improvement of sur- 5.2. Accelerating the process rate
face functional groups of the biochar can be achieved by an
oxidation process (Kumar et al., 2020b,c), yet the oxidation pro- The start-up potential of an AD system can be significantly
cedure should be adequate to acquaint with new functionalities but accelerated with the addition of biochar. As illustrated by
not too strong to induce transformation to the redox-inactive COOH Shanmugam et al. (2018), a 24-h reduction in the lag phase of
functional group or even elimination as CO2 (Chaco
n et al., 2020). methanogenic microbe during the AD of wastewater was achieved
Free radicals affect the redox tendency of biochar, such as aryl using biochar derived from algal biomass via hydrothermal
radicals (carbon-centred) or as semi-quinoid radicals (intermediate carbonization. This finding corroborated previous results that the
of the phenolic CeOH and quinoid C]O groups) (Joseph et al., biochar to substrate (citrus peel) ratio was inversely proportional to
2015). Regarding the inorganic components of biochar, redox- the duration of microbial lag phase, and the optimized ratio
active metals such as Fe and Mn oxides are generally present in resulted in the shortest lag phase of 7.5 days (Fagbohungbe et al.,
the feedstock and exist in an array of different oxidation states that 2016). Similarly, the addition of biochar reduced the lag phase of
can serve as electron donors and acceptors (Dieguez-Alonso et al., CH4 and H2 reactor by 41e45% and 21.4e35.7%, respectively
2019). Their degree of involvement in the EEC depends on the (Sunyoto et al., 2016). The lag phase was completely avoided by the
metal types, variations in the oxidation states, distribution of the addition of biochar or shortened by 0.9e1.83 days by adding
metal oxides, and the coordination as organo-mineral complexes magnetic biochar during methanogenesis (Viggi et al., 2017; Qin
on the biochar surface (Park et al., 2018; Ren et al., 2020). et al., 2017). Moreover, Wang et al. (2018a) observed a decrease
It was revealed that, due to conductive properties, biochar could from 4.7 days to 1.8e3.9 days in the lag phase of co-digestion of SS
facilitate DIET during the AD process in co-cultures of Geobacter and FW with biochar application. The CH4 daily yield increased by
metallireducens with Geobacter sulfurreducens or Methanosarcina 136% after the amendment of wood-pellet biochar in the AD pro-
barkeri in a similar manner as GAC (Chen et al., 2014b). The solid cess (Indren et al., 2020). The CH4 production also rose by 1.6 times
biochar and its soluble fraction displayed better DIET promotion after co-digestion of FW and WAS at the higher substrate to
9
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Fig. 4. Schematic illustration of the roles of biochar in AD process.

inoculum ratios (2.5e3 and 3.9e5.0) with biochar addition (Viggi properties of biochar and variable operating parameters of the AD
et al., 2017; Li et al., 2018). In a yearlong evaluation of Shen et al. process.
(2017), not only the CH4 production rate but its volume concen-
tration increased in a semi-continuous AD. Jang et al. (2018)
5.4. Inhibitors adsorption
observed that the biochar (10 g L1) amendment at variable tem-
peratures (20, 35, and 55  C) in the AD elevated the CH4 yield by
One of the prime features offered by biochar to elevate AD
27.7e35.7%. Sunyoto et al. (2016) also recorded a 23e41.6% and
functioning is its inhibitors adsorption potency (Table 4). Thea ar-
1.9e9.6% increase in the CH4 production with biochar addition in a
omatic structures of biochar facilitates p-p interaction for the
two-phase AD system.
adsorption process, which is supplemented by the existence of OH
and COOH groups (Kanjanarong et al., 2017). Tan et al. (2017)
pointed out the significance of functional groups over pore size
5.3. Buffering potency and alkalinity
for the hydrochar adsorption. According to Shanmugam et al.
(2018) and Cheng et al. (2018), CH4 yield was elevated due to bio-
The effectiveness of an AD system is primarily dependent upon
char adsorption of VFAs and acid alleviation. Wang et al. (2018a)
the pH value, where a drop in the solution pH significantly hampers
observed a direct proportionality between hydrochar SSA and
microbial functioning (Qiu et al., 2019). High biodegradability and
NHþ 4 -N adsorption. Xu et al. (2018) reported adsorption of 25 mg of
low C:N ratio of FW, resulting in a fast acidification rate in the AD
NH₄⁺ and 50 mg of VFAs by 1 g hydrochar in the pig carcass AD.
process. The rapid proliferation of acidogenic bacteria in the
Moreover, Linville et al. (2017) evaluated walnut shell biochar in the
acidogenesis stage will hinder the activity of methanogens and lead
AD of FW (thermophilic and mesophilic conditions) and observed
to the accumulation of VFAs (Ren et al., 2018). Earlier studies
effective CO2 removal by smaller (61%) and coarser biochar (51%). In
confirmed that this situation might occur in the case of excessive
two-stage digesters of AD of WAS using biochars from pine wood
organic loadings with readily biodegradable substrates (Fotidis
and corn stover, Shen et al. (2017) reported 81e88.6% and
et al., 2013). As there is a long recovery time of the AD system
72.1e76.6% CH4 contents in the corn stover and pinewood biochar
from accumulated VFAs, biochar addition can serve as a quick and
amended reactor in comparison to 70.0% in control. The biochar
simple method to accelerate the recuperation of acidified anaerobic
released base cations could sequester CO2 into carbonate/bicar-
reactors (Ren et al., 2020). Wang et al. (2018a) and Jang et al. (2018)
bonate. There were two controlling factors of biochar at work,
highlighted the importance of biochar pH buffering capacity and
adsorption of CO2 and syntrophic support of CO2 reducing metha-
nutrient availability in the co-digestion system of SS, FW, and dairy
nogens and organic acid oxidizing bacteria on the biochar
waste. Sunyoto et al. (2017) showed that biochar addition could
(Masebinu et al., 2019; Pan et al., 2019).
supply nutrients to a two-phase AD of carbohydrate FW and assist
the pH stabilization.
Nonetheless, there are some contradictory findings against the 5.5. Enriched microbial functionality
potential application of biochar in the AD process. Luo et al. (2015)
suggested that acid inhibition might occur before CH4 production in Zhang et al. (2017) reported an interesting observation that
the AD of synthetic wastewater, and biochar could not significantly during the biofilm formation, biochar induced the secretion of
increase the pH buffering capacity. Sunyoto et al. (2016) observed a extracellular polymeric substance (EPS) from microbes, thus facil-
notable drop in pH value from 5.0 to 3.0 due to VFAs accumulation itating microbial adhesion on the biochar surface. This presents a
even in a biochar-amended AD. Besides, hydrochar containing hu- simple and low-cost solution using biochar to avoid rapid sludge
mic acid might accelerate sludge solubilization and acidification granulation and minimize loss of methanogens in the anaerobic
(Wang et al., 2017b; Zhang et al., 2014c). There is no definite digesters. Sun et al. (2016) confirmed the enriched microbial
conclusion regarding the pH buffering capacity of biochar addition abundance in the presence of biochar carrier. Dang et al. (2016)
in the AD system, which depends on different physicochemical revealed that biochar improved the capacity of enriched
10
 Table 3

M. Kumar, S. Dutta, S. You et al.

Application of biochar as additives in the production of CH4 using FW, sludge, and FW þ sludge as feedstock.

AD Feedstock AD Reactor Biochar Biochar OLR Pre-treatment Enriched microorganism Identification CH4 yield Highlights of the study Reference
Conditions Feedstock Condition technologies
(T, pH, (T, pH)
Days)

FW T ¼ 38, Batch Sludge T ¼ 350, _ _ _ _ 285.7 mL g1 COD Evaluation of CH4 production using Ambaye et al.
pH ¼ 7.1 550, fruit waste as feedstock and SS and (2020)
pH ¼ 6.4, biochar as additives.
9.5
WAS þ PS þ Fat T ¼ 55, Batch Sludge T ¼ 800 _ _ _ _ 240 ± 24 mL g1 VS Anaerobic co-digestion confirmed Gonza
lez-
that the addition of 3% (w/v) of fat to Arias et al.
the feeding sludge results in a 25% (2020)
increment in electricity generation
from biogas.
Sludge T ¼ 37, _ Corn stover T ¼ 500, _ _ M. harundinacea _ 260.5e342.1 mL g1 Two different biochar (pyrolyzed and Zhou et al.
pH ¼ 8.2, pH ¼ 2 VS H2SO4 treated) applied for the (2020)
D ¼ 23 production of biogas. This finding
stabilizes the role of biochar
properties on AD operation.
FW T ¼ 55, Batch Wood pellets T ¼ 700- 1.52 _ Defluviitoga, Illumina 0.465e0.543 L g1 VS Impact of biochar with varying Zhang et al.
pH ¼ 7.41, 800 e3.04, Methanothermobacter and Hiseq 2000 (Increased by 18%) particle sizes at a model dosage of (2020b)
D ¼ 15 4.56, Methanosarcina 15 g L1 at AD in semi-continuous
6.08, bioreactor.
9.12 g VS
L1 d1
Sludge T ¼ 55, Batch Waste forest T ¼ 450 _ _ _ _ 328 ± 7 mL g1 COD Powdered biochar dosage improves Cimon et al.
pH ¼ 7.6 e550, the CH4 production rate from 192 to (2020)
e8.4, 461% in the first 16 days.
11

D ¼ 19-49
Sludge T ¼ 55, _ Corn stover T ¼ 600, _ _ Proteobacteria, Bacteroidetes, _ 341 mL g1 VS Biochar amendment in digester Wei et al.
pH ¼ 7.7 pH ¼ 10.1 Firmicutes, Acidobacteria, upgraded CH4 content from 67.5% to (2020)
87.3% and enhanced CH4 production
from 8.6 to 17.8%.
Sludge T ¼ 37, Batch Sludge T ¼ 400 _ _ Methanothermobacter, _ 172.3 mL g1 COD The maximum CH4 yield achieved Wang et al.
pH ¼ 7.9, e600, Methanosarcina, with DF500 (biochar from Douglas fir (2020a)
D ¼ 30 pH ¼ 5.61 Methanomassilii- coccus at 500  C), which was about 48.3%
e6.13 more than control.
FW þ algal T ¼ 35, 55, Batch Algal biomass T ¼ 500- 3.21 g _ Firmicutes, Bacteroidete, Illumina 299.7e536.6 mL g1 During semi-continuous co-digestion Zhang et al.
biomass pH ¼ 7, 600 VSL1d1 Methanofastidiosum, Hiseq 2000 VS of 25% FW and 75% algal biomass (2020a)
D ¼ 45 Methanosaeta, mixture, amended with biochar leads
Methanospirillum to 12e54% CH4 increment in
comparison to control.
FW þ Sludge T ¼ 35, Batch Saw dust T ¼ 300- 1.1e3.5 g _ Petrimonas, Methanosarcina Illumina 373e452 mL g1 VS Biochar prepared at 500  C achieved Wang et al.

Journal of Cleaner Production 305 (2021) 127143

pH ¼ 7.3 700 VS L1 Miseq PE250 better CH4 yield than others biochar (2020c)
e8.2 d1 prepared at different temperature.
Electrochemical analysis revealed the
outstanding electron transfer
capacity of biochar, which facilitate
methanogenesis.
Sludge T ¼ 55, Batch Cow dung, T ¼ 350 _ _ _ _ Increased by 133.7% Three sewage sludge char (SSC) and Yue et al.
pH ¼ 8, sewage sludge e600, biochar could enhance cumulative (2019)
D ¼ 26 pH ¼ 6.8 CH4 production from 120.7 to 133.7%.
e11
FW T ¼ 35e37, _ Commercial T ¼ 500, 6.0 g VS _ Methanothri, _ _ Both municipal sludge biochar and Giwa et al.
pH ¼ 5.5 biochar (CBC) pH ¼ 7.85 L1 d1 Methanobacterium and commercial biochar (CBC) exhibited (2019)
e6.7 and e9.01 Methanomethylovorans comparable efficiency and improved
CH4 yield (5%)
(continued on next page)
 Table 3 (continued )

M. Kumar, S. Dutta, S. You et al.

AD Feedstock AD Reactor Biochar Biochar OLR Pre-treatment Enriched microorganism Identification CH4 yield Highlights of the study Reference
Conditions Feedstock Condition technologies
(T, pH, (T, pH)
Days)

municipal
sludge
Sludge T ¼ 35, Batch Corn straws T ¼ 600 _ _ Methanobacter _ 118.29 ± 4.35 L kg1 Manganese oxide-modified biochar Li et al. (2019)
pH ¼ 6.5, VS composite (MBC) could increase the
D ¼ 34 buffering capacity, facilitate
degradation of intermediate acids,
buffer the pH of the culture, stabilize
the SS AD process, and CH4 yield
increased up to 121.97%, as compared
to control.
Sludge T ¼ 37, Batch Sludge T ¼ 300- _ _ Syntrophomonas, _ 132.04 ± 4.41 mL g1 Hydrochar encouraged CH4 Wu et al.
pH ¼ 7.1, 700 Peptococcaceae, VS production compared with pyrochar. (2019)
D ¼ 32 Methanosaeta and The highest cumulative CH4 yield
Methanobacterium obtained with the addition of
hydrochar produced at 180  C. In
contrast, the pyropchar synthesized
at 500 and 700  C exhibited a slight
adverse impact on CH4 yield.
FW þ Sludge T ¼ 35, 55 Batch Pine T ¼ 800 _ _ Methanothermobacter, Illumina 829.0e681.0 mL g1 Powdered biochar enriched the Lü et al.
Methanolinea Miseq PE250 VS microbial communities and further (2019)
improved CH4 yield by 13.3% in
thermophilic conditions.
FW T ¼ 37, Batch Plant Biomass T ¼ 450 _ _ _ _ 46e540.4 This study presented a novel Luz et al.
pH ¼ 7 (Ampelodesmos e550, mL g1 VS approach which possibly combines (2018b)
12

e7.5, mauritanicus) phytoremediation and generation of

D ¼ 15 biomethane using Ampelodesmos
mauritanicus as biochar feedstock.
FW þ Sludge T ¼ 55, Batch Sawdust T ¼ 500 _ Thermal Firmicutes, Thermotogae, Illumina 200 mL g1 VS Biochar amendment dramatically Li et al. (2018)
pH ¼ 5e8, Methanospirillum, high- reduced the lag phase and improved
D ¼ 28 Methanosaeta throughput CH4 yield.
sequencing
(HTS)
FW þ Sludge T ¼ 35e37, Batch Sludge _ 1.49 _ Clostridium, Eubacterium, Illumina-HTS 318e500 L kg1 VS Biochar had a positive impact in Martínez
pH ¼ 7.6, e4.48 kg Geobacter, Anaerolineaceae, batch digestions, leading to a reduced et al. (2018)
D ¼ 30 VS Methanosaeta in the lag phase and an improved in
L3 d1 CH4 yields.
Sludge T ¼ 37, UASB Agricultural _ _ Thermochemical Saccharofermentants, Illumina Increased by 68.1% Biochar played a significant role in Zhuang et al.
pH ¼ 7, waste Comamonas, Alipia, Miseq the removal of COD, improvement in (2018)
D ¼ 30 Methanosaeta, CH4 yield, and VFA reduction by

Journal of Cleaner Production 305 (2021) 127143

Methanosarcina 37.5% than control.
FW þ Sludge T ¼ 35, UASB and Sawdust T ¼ 500, 0.4 kg _ Methanothrix, Geobacter Illumina Increased by 11% Amendment of biochar leads in the Wang et al.
pH ¼ 7.1 batch pH ¼ 10.58 e15 kg MiSeq reduction of the lag phase of (2018a)
reactors COD m3 methanogenesis by 28.6%, and the
d1 strengthening factor of COD removal
rate reached 1.6.
Sludge T ¼ 35, Batch Sawdust T ¼ 500 0.75, 1.5, _ Anaerolineaceae, Illumina Increased in In comparison to control, biochar Wang et al.
pH ¼ 7.6, 2.25 g VS Methanosaeta, Miseq PE250 production rate from amendement effectively shortened (2018b)
D ¼ 12 L1 d1 Methanobacterium and 22.4% to 40.3% the lag time by 27.5e64.4% and
Methanolinea increased the CH4 yield.
FW T ¼ 35, Batch Vermicompost T ¼ 500, _ e _ _ _ AD of chicken manure did not occur Wang et al.
pH ¼ 6.8, pH ¼ 7.83 at higher organic loading of 50 g TS (2017a)
D ¼ 25 kg1, while it worked well with 5.0%
vermicompost biochar or
untransformed vermicompost.
 M. Kumar, S. Dutta, S. You et al.
FW T ¼ 20, Batch Wheat bran T ¼ 500 _ _ Methanosaeta, _ _ CH4 production proceeded at a rate Viggi et al.
pH ¼ 7 pellets, e800, Methanosarcina up to 5 times higher than control. (2017)
coppiced pH ¼ 7.5 Biochar increased electron transfer
woodlands, mechanism during AD.
orchard
pruning
Sludge T ¼ 35, _ Rice straw and T ¼ 500 _ _ Methanosarcina, Illumina 194.6 mL g1 VS Magnetic biochar treatment on AD Qin et al.
pH ¼ 7.5 FeCl3 Methanobacterium, Miseq PE250 resulted in 38.34% reduction in CH4 (2017)
e7.8, Methanosaeta yield, due to competition of iron
D ¼ 25 oxide for electrons.
FW þ Sludge T ¼ 37 or Batch Walnut shell T ¼ 900 _ Thermal _ _ 492-600 mL g1 VS Average CH4 volume concentration in Linville et al.
55, biogas improved up to 98.1%, with (2017)
pH ¼ 7.4 finer biochar than coarser biochar
e8.6,
D ¼ 26-54
Sludge T ¼ 55, Semi- Corn stove, _ 0.24 Thermal _ Illumina Increasedproduction Both corn stove biochar and pine Shen et al.
D ¼ 30 continuous pine e0.72 g HiSeq2000 rate up to 25%e37%. biochar promoted the substrate (2017)
VS L1 and MiSeq utilization, CH4 productivity, and
d1 process stability of AD.
Sludge T ¼ 32, Batch Bamboo _ 6 kg COD _ Methanosaeta, Illumina 0.25e0.35 L g1 COD Enhance COD removal efficiency. Xia et al.
pH ¼ 6.8 m3 d1 Methanospirillum, and MiSeq (2016)
e7.2, Methanobacterium
FW T ¼ 40, Batch Holm oak T ¼ 650, _ _ _ _ 279.8 mL g1 VS Biochar was established with a setup Meyer-
D ¼ 30 pH ¼ 10.3 that imitated at large-scale biogas Kohlstock
plant. Both biogas and CH4 yield et al. (2016)
improved around 5% with biochar.
FW T ¼ 35, Batch Pine sawdust T ¼ 650, _ _ _ _ Increased in Biochar amendment shortened the Sunyoto et al.
pH ¼ 7 production rate by lag phases along with enhanced VFA (2016)
23.0%e41.6% degradation in CH4 production.
FW T ¼ 35, Batch Fruitwoods T ¼ 800 _ _ _ _ _ At I:S ¼ 2, 1, and 0.8 shortened the lag Cai et al.
13

pH ¼ 7 e900, phase of digestion by 20.0e10.9%, (2016)

pH ¼ 8.6 43.3e54.4%, and 36.3e54.0%, and
raised the maximum CH4 production
rate by 100e275%, 100e133.3%, and
33.3e100%, respectively in
comparison to control.
Sludge T ¼ 34, _ Pinewood T ¼ 650 0.75 _ Methanomicrobiales, _ 620 mL and Carbon felt and biochar, both De Vrieze
pH ¼ 68.3, e2.0 g Methanosaetaceae 640 mL L1 d1 materials facilitate stabilization of AD et al. (2016)
D ¼ 20 COD process and active enrichment of the
L1 d1 methanogenic
FW T ¼ 35, _ Wood T ¼ 450, 0.4e1.6 g _ _ _ 163.9e186.8 mL g1 Biochar reduced lag phase duration Fagbohungbe
pH ¼ 6e8, coconut shell, pH ¼ 8.3 VS L1 VS and parallelly enhanced CH4 yield. et al. (2016)
D ¼ 30 rice husk d1
Sludge T ¼ 37e55, Batch Corn stover T ¼ 600 _ Thermal _ _ Increase up to 7 The Biochar addition enhanced the Shen et al.
pH ¼ 7.5 e27.6%. CH4 yield. (2015)

Journal of Cleaner Production 305 (2021) 127143

e9, D ¼ 30
FW T ¼ 42 Batch Paper sludge T ¼ 500 _ _ _ _ Increased by 32% For pyrochar, no significant effect on Mumme et al.
and wheat biogas production was observed, (2014)
husks whereas hydrochar increased the
methane yield by 32%. This correlates
with the hydrochar’s larger fraction
of anaerobically degradable carbon
(10.4% of total carbon, pyrochar:
0.6%).
Sludge T ¼ 35, Two Japanese cedar _ 2.17 g _ Methanosaeta, _ 1.6-time increment Stable CH4, production rate. Watanabe
D ¼ 30, single-step COD Methanoregula,Methanocellus et al. (2013)
reactors L1 d1
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Table 4
NHþ4 , H2S and CO2 adsorption capacity of different biochar.

Biochar production Biochar properties Adsorption Reference

Feedstock Pyrolysis Surface pH CEC Total Source of Initial NHþ þ

4 NH4 Adsorption capacity Inlet H2S or H2S CO2
temperature area (cmol pore NHþ4 -N (mg L1) (NHþ4 -Ng
1
mg biochar) CO2 Adsorption Adsorption
( C) (m2g1) kg1) volume concentration capacity capacity
(mmol (mmol g1)
g1)

Municipal 400e450 e 9.5 65.7 e NHþ4 1000 137.3 e e e Takaya et al.

waste ±16.2 solution (2016)
Municipal 600e650 e 10.2 67.9±12.5 e NHþ4 1000 128.3 ±6.7 e e e Takaya et al.
waste solution (2016)
Corncobs 600 23 8.92 0.098 AD slurry 500e580 108.9 e e e Kizito et al.
[mL g1] (2016)
SS 500 71.6 e e e e e e 1% (v/v) 1.29 e Xu et al.
(2014)
Potato 500 63 e e e e e e 1000 ppm 1.56 e Sun et al.
peel (2017)
waste
Perilla leaf 700 473.4 e e 0.1 e e e e 0.54 2.312 Sethupathi
[cm3g1] et al. (2017)
SS 500 10.12 e e 0.022 e e e e e 0.41 Xu et al.
[cm3g1] (2016)

Enterococcus and Sporanaerobacter, which could possibly break 2018). Fick’s Law governs the microbial metabolite exchange
down fermentable substrates to transfer the generated electrons to occurring through diffusion: the distance is inversely proportional
Methanosarcina (which was also enriched with the biochar addi- to microbial metabolite flux. Therefore, once the cell accumulation
tion) (Table 5). Methanosaetaceae and Methanosarcinales could form is achieved, anaerobic bacteria elevate the rate of interspecies
biological interactions with the added biochar and effectively hydrogen transfer, and compact structures are developed by
decrease the lag time (Lü et al., 2016). methanogenic archaea behaving as an organ (Chiappero et al.,
Wang et al. (2018a) observed that hydrochar dosage is directly 2020). On the other hand, IIET and soluble metabolites diffusion
proportional to the ease of methanogenic bacteria attachment. A is regarded as a bottleneck in CH4 production by slowing down the
similar result was recently reported for acetoclastic methanogen electron transfer mechanism and energy transfer (Lovley, 2017;
Methanosaeta enrichment with hydrochar addition (Ren et al., Park et al., 2018). In contrast, DIET does not require the electron
2020). Hence, CH4 production from VFAs could be promoted by shuttle mediation for an electric current generation between
methanogens immobilization by the added hydrochar (Xu et al., electron-accepting and donating microbes (Martins et al., 2018).
2018). Moreover, biochar could promote biofilm formation and Compared to IIET, DIET was reported to be more specific and faster
achieve functional enrichment of microbes for AD enhancement (Lovley, 2017; Summers et al., 2010). According to Park et al. (2018),
(Yin et al., 2019). In correspondence with the biochar pore size exchange of direct electron through microbial pili was detected in
(1e40 mm) (Huggins et al., 2016), its pores can contain 2e10 co-cultures of Geobacter sulfurreducens and G. metalliriducens
methanogenic cells (Lü et al., 2016). Therefore, it is important to (Summers et al., 2010), Methanosarcina barkeri (Rotaru et al.,
choose appropriate biochar with favourable pore size distribution 2014a), or Methanosaeta harundinacea (Rotaru et al., 2014b). DIET
for biofilm formation (Zhang et al., 2017). The microbial could be efficiently mediated between syntrophic partners via
morphology is also an essential parameter (Lü et al., 2016). For different conductive materials such as GAC (Liu et al., 2012), biochar
example, the addition of biochar accelerated the attachment of (Chen et al., 2014b), and magnetite (Liu et al., 2015).
Methanoculleus and Methanosaeta to the internal porous layer and While considering the microbial community composition, AD
Methanosarcina to the external surface of biochar matrix (Tang elevation has been validated by DIET (conductive biochar) and the
et al., 2020). enhancement of formate and H2 interspecies transfer mechanisms
(Fig. 5). Martínez et al. (2018) observed that co-culture generation
5.6. Electron transfer mechanism promoted CH4 production, for example, homoacetogenic bacterial
enrichment including Eubacterium, Clostridium, Syntrophomonas,
Previous studies also highlighted the importance of biochar and H2 with methanogens. Zhao et al. (2016) investigated the se-
addition to its capability of electron transfer processes between lective enrichment of Methanosaeta and Geobacter on biochar in
archaea and anaerobic bacteria (Table 5). The efficiency of the AD synthetic wastewater AD with propionate and butyrate, where
system is primarily dependent upon the syntrophic interactions DIET could degrade propionate and butyrate in the presence of
between methanogens and bacteria, which trade electrons to conductive biochar and an abundance of Smithella and Syntropho-
comply with their energy necessities (Martins et al., 2018). This monas confirmed the interspecies electron transfer mechanism.
occurs through multiple routes: DIET via a conductive medium Wang et al. (2018a) studied microbial abundance in the biochar-
(e.g., GAC, magnetite, carbon cloth, biochar) (Zhang et al., 2018), amended reactor for synthetic wastewater AD and reported selec-
membrane-bound transporter proteins (Martins et al., 2018), tive improvement of potential DIET-associates such as Bacter-
electric conductive pili (Barua and Dhar, 2017), and indirect inter- oidetes, Geobacter and archaea Methanosarcina and Methanosaeta.
species electron transfer (IIET) through insoluble (humic com- The biochar showed the potency to elevate DIET among electro-
pounds) (Roden et al., 2010) and soluble (acetate, formate, genic archaea and microbes, thus enhancing COD removal and
hydrogen) substances (McGlynn et al., 2015; Schink et al., 2017). electron transfer features of granular sludge and CH4 yield. Wang
Formate and hydrogen in IIET function as electron shuttles amid et al. (2018b) observed that biochar addition in variable doses led
methanogens and syntrophic-producing bacteria (Martins et al., to higher CH4 generation and reduced lag time in the mesophilic AD

14
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Table 5
Impact of biochar on microbial communities in AD processes.

Biochar Biochar synthesis Biochar Substrate Inoculum Reactor Experimental Possible Results Reference
feedstock condition dose T ( C) mode/ mechanisms
conditions

Macadamia Pyrolysis; T ¼ 350  C; 33.3 g L1 FW þ water Digestate from UASB 37 CIC reactor; Decreases NH3 Increased Su et al.
nutshells D ¼ 2 h; þ increasing N (SS ¼ 34 g L1) V ¼ 4.6 L; inhibition; COD (2019)
HR ¼ 10  C min1 eNH4 dosage HRT ¼ 16 h increases alkalinity; removal by
decreases VFAs 15%
accumulation;
increases selective
enrichment of
functional
microbes,
acclimatization and
attachment on
biochar.
Sawdust Pyrolysis; 15 g L1 FW Anaerobic digestate 55 Semi- Increases VFAs Increased Wang et al.
T ¼ 500  C þ SS (TS (TS ¼ 5.2%) continuous; syntrophic CH4 yield by (2019)
¼ 9.2%); Serum bottles; oxidation; increases 16.0%
FW:Sludge ¼ 4:1 WV ¼ 150 mL; microbial e55.2%;
(TS) Decreasing attachment; Stable CH4
HRT; increases production
increasing OLR association with at increasing
syntrophic OLRs
partners;
stimulating DIET.
Sawdust Pyrolysis; T ¼ 500  C; 10 g L1 FW WAS (TS ¼ 89.1 g L1) 55 Batch; Increases buffer Increased Li et al. (2018)
D ¼ 1 h; (TS ¼ 94.2 g L1) V ¼ 120 mL; capacity; OLR:
HR ¼ 20  C min1 S:I (VS) ¼ 0.25 increases microbial Decreased
e3 attachment and lag time;
acclimation on Increased
biochar; CH4
increases DIET; production
increases rate
enrichment of
selective microbial
communities.
Sawdust Pyrolysis; 2e15 g L1 Dewatered WAS Anaerobic digestate 35 Batch; Increases buffer Decreased Wang et al.
T ¼ 500  C; þ FW (TS ¼ from a brewery Serum bottles; capacity; increases lag phase by (2018b)
D ¼ 1.5 h; 8.8%) factory (TS ¼ 6.8%) WV ¼ 90 mL; DIET due to the 27.5e64.4%;
HR ¼ 10  C min1 þ water S:I ¼ 0.75e3 richness of surface Increased
(VS) functional groups maximum
on biochar; CH4
Selective production
enrichment of rate by
microbial DIET- 22.4%
partners e40.3%
Vineyard Pyrolysis; T ¼ 500  C 10 g L1, Co-digestion: WWTP anaerobic 37 Batch; Promote syntrophic Decreased (Martínez
prunings 30 g L1 Orange peels digestate V ¼ 250 mL; metabolism; lag phase; et al., 2018;
(TS ¼ 311 g kg ); (TS ¼ 35.5 g kg1)
1
Semi- adsorption of Increased Rosas et al.,
SS continuous; inhibitors; CH4 2015)
(TS ¼ 28.7 g kg1) V ¼ 3 L; adhesion and production.
HRT ¼ 10e30 growth of
days microorganisms on
biochar surface.
Wheat bran Pyrolysis; 25 g L1 FW digested Methanogenic 20 Batch; No effects on pH; Increased Viggi et al.
pellets T ¼ 800  C; culture V ¼ 120 mL no effects on NH3 VFAs (2017)
D ¼ 3h (from WAS digestate) adsorption; degradation
promote IET. rate;
reduced lag
phase.
Rice Carbonization; 0.5% w/w SS þ water OFMSW þ anaerobic 35 Batch; no effects on NH3 Decreased Qin et al.
straw þ FeCl3 T ¼ 500  C; (TS ¼ 1.64%) digestate þ water Serum bottles; adsorption; lag phase; (2017)
D ¼ 2h (TS ¼ 2.19%) V ¼ 500 mL; no effects on pH; Increased
S:I ¼ 1 (VS) increases CH4
syntrophic production
associations of by 11.69%
bacteria on biochar
surface;
increases DIET.
Pine sawdust Pyrolysis; 8.3 FW (bread) WWTP-sludge 35 Batch; Increase Decreased Sunyoto et al.
T ¼ 650  C; e33.3 g L1 (TS ¼ 61.2%) (heated at V ¼ 100 mL; methanogenic lag phase; (2016)
D ¼ 20 min 95  C) biofilm formation; Increased
increases VFAs
availability of generation
(continued on next page)

15
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Table 5 (continued )

Biochar Biochar synthesis Biochar Substrate Inoculum Reactor Experimental Possible Results Reference
feedstock condition dose T ( C) mode/ mechanisms
conditions

nutrients; and
increases pH degradation;
buffering capacity. Increased H2
and CH4
production
rate.
Coconut shell Pyrolysis; 1:1 (TS) Citrus peel WWTP anaerobic 55 Batch; Increases Reduced lag Fagbohungbe
T ¼ 450  C (TS ¼ 16.6%) digestate V ¼ 500 mL contaminate phase; et al. (2016)
(TS ¼ 11.0%) S:I ¼ 0.31 adsorption. Increased
e0.33 (VS) AD stability;
CH4
production.
Corn stover Gasification 1.82 WWTP sludge WWTP anaerobic 55 Batch; Increases buffer Increased Shen et al.
e3.64 g; digestate V ¼ 600 mL capacity; CH4 (2015)
BC g-1 increases electrical production
Total conductivity; (88.5
sludge increase e96.7%).
solid (TSS) extracellular
electron transfer;
reduces NH3
inhibition;
increases CO2
sequestration;
increases
availability of
macro-/micro-
nutrients.
Corn stover Gasification ¼ 850  C 0.25 PSþ WWTP anaerobic 55 Semi- Adsorption and Increased (Cheah et al.,
e1.0 g d1 WAS (TS ¼ 7.01%) digestate (TS ¼ 3.77 continuous precipitation of CH4 2014; Shen
e6.14%) V ¼ 500 mL CO2; decreases production et al., 2017)
TPAD: TAN; (13.7
1) HRT ¼ 5, 15 increased e25.3%) and
and 13e30 alkalinity; production
days. increased macro-/ rate by 5.5
micro-nutrients in e36.9%.
digestate;
change in bacterial
community
diversity.

of dewatered WAS along with FW. biochar prepared from 32 g FeCl3: 100 g rice-straw impeded CH4
Recently, Akturk and Demirer (2020) found that 2.0 g L1 and production and decreased CH4 yield by 38.3%, probably due to the
5.0 g L1 biochar could improve the CH4 yield by 11.2 ± 6.5% and competition between iron oxides (excessive amount in the mag-
27.3 ± 9.5%, respectively. The application of Fe-functionalized bio- netic biochar) and DIET microbes for electrons (Qin et al., 2017). Up
char also significantly improved the efficacy of the DIET mechanism to now, the research on the mechanism of microbial DIET is still in
(Qin et al., 2017). The magnetic biochar synthesized from 3.2 g an infancy stage, and the science-informed production of biochar as
FeCl3: 100 g rice-straw improved CH4 yield by 11.7%, while the an additive is yet to be optimized.

6. Techno-economic and life cycle analysis

In comparison to composting, the use of FW as feedstock for the

generation of bioenergy at the commercial level have the advan-
tages of low carbon emissions, less secondary pollution generation,
low operational costs, and less global warming potential (GWP) (Li
et al., 2019b). Oldfield et al. (2016) reported that AD had a minimum
environmental impact and the highest gain of carbon credit
compared to incineration and composting.

6.1. Techno-economic analysis

Sahoo et al. (2019) and Harsono et al. (2013) performed an

economic assessment on biochar generation from lignocellulosic
feedstock to evaluate the investment costs, which could be
balanced by a 470 V t1 biochar trade price. It is important to
realize that extending AD applications towards unconventional
substrates would provide additional financial incentives, which
Fig. 5. Schematic illustration of DIET mechanism via biochar. should be supplemented with the higher yield of CH4 and
16
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

Table 6
Production cost of biochar using various cost-effective feedstocks.

Biochar Feedstock Production process Scale Production Cost (USD kg1) Country Year Reference

Short rotation coppicing Slow Pyrolysis small 0.434 UK 2015 Lehmann and Joseph (2015)
Forestry residue Slow Pyrolysis large 0.345 UK 2015 Lehmann and Joseph (2015)
Forestry residue Slow Pyrolysis medium 0.584 UK 2015 Lehmann and Joseph (2015)
Pine wood Slow Pyrolysis medium 0.220e0.280 USA 2014 Shabangu et al. (2014)
Straw Slow Pyrolysis medium 0.447 UK 2015 Lehmann and Joseph (2015)
Straw Slow Pyrolysis small 0.351 UK 2015 Lehmann and Joseph (2015)
Empty fruit bunches Slow Pyrolysis small 0.533 Malaysia 2013 Harsono et al. (2013)
Short rotation coppicing, forestry residues, short rotation forestry Slow Pyrolysis large 0.266 UK 2015 Lehmann and Joseph (2015)
Short rotation coppicing, forestry residues, short rotation forestry Slow Pyrolysis medium 0.5 UK 2015 Lehmann and Joseph (2015)
Straw Slow Pyrolysis large 0.203 UK 2015 Lehmann and Joseph (2015)
Arboricultural arisings Pine Slow Pyrolysis small 0.213 UK 2015 Lehmann and Joseph (2015)

associated energy. The addition of biological and inorganic ele- material flow. Qiu et al. (2019) recommended the energy
ments such as micronutrients and iron is commonly employed to investment-generation LCA technique to estimate the energy
enhance CH4 production. For instance, 13e16 V L1 nutrients and linked with AD components to evaluate the total energy input and
3.60e4.10 V L1 enzyme are added to elevate the AD applications as energy investment return from biogas production.
additives (ICIS, 2018). Compared to GAC (0.6 and 20 $ kg1), the
overall production costs of biochar are reasonable (0.2e0.5 $ kg1) 6.2. Life cycle analysis (LCA)
depending upon factors such as the pyrolysis process and feedstock
(Table 6). Furthermore, compared to AD alone, integration of FW A net gain in energy was reported for biochar production
and sludge AD with digestate pyrolysis/hydrothermal carboniza- through pyrolysis of empty fruit bunches of palm oil (Harsono et al.,
tion can boost the net energy generation and elevate its soil 2013). A positive energy balance was recorded during the genera-
amendment quality with environmental and economic advantages tion of biochar from multiple lignocellulosic materials in LCA
(Antoniou et al., 2019). (cradle to grave approach) (Moreira et al., 2017), which is advan-
Recently, Peng and Pivato (2019) applied a back to earth alter- tageous from environmental and economic perspectives. LCA of
native and circular economy model to manage the digestate biochar production from lignocellulosic feedstock revealed GHGs
generated from AD of FW and organic fraction of MSW. The inte- emissions for organic waste, straw and wood between 20 and 50 g
gration of biochar-based AD and the recycling of remaining diges- CO2-eq MJ1, whilst for pit/shell/husk, the emission varied between
tate for the synthesis of biochar via pyrolysis/gasification for its 120 and 250 g CO2-eq MJ1 (Li et al., 2017b). Feedstock having an
subsequent application in AD could realize complete resource uti- ash content 0e2% and a high O:C ratio was associated with higher
lization and close the material loop. Opatokun et al. (2016) used FW GHGs emissions (Sharifzadeh et al., 2019). Different scenarios were
and its digestate for biochar synthesis to generate energy, fuel, evaluated (GREET, 2018) to demonstrate that there was 85e98%
biofertilizer, and chemical for industries. Similarly, Hung et al. reduction in GHGs emissions from lignocellulosic biomass in
(2017) used AD digestate to fabricate porous biochar and demon- comparison to petroleum fuels, equivalent to 93 g CO2-eq MJ1. This
strated multifunctional applications of biochar as biofertilizer, reduction in GHGs emission aids to comply with 50% stake of
adsorbent, and soil amendments for establishing a closed-loop renewable energy standard for GHGs release reduction prerequisite

Fig. 6. Integrated approach for the production of engineered biochar and biorenewable energy from food waste and sludge.

17
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

for unconventional fuels (Chiappero et al., 2020).  Previous investigations demonstrated the efficacy of the fed-
During the investigation of carbon equivalent abatement (CA) of batch biochar-amended AD system, while further investigation
biochar production processes, maximum electricity generation efforts should be paid to its application in a continuous/semi-
output (0.9 MWhe t1 of biomass) was observed for gasification, continuous anaerobic process and its recycling and reuse.
while maximum CA was observed for pyrolysis (0.07e1.25 t CO2-eq  Prudent procedures should be developed to avoid the inhibition
t1 feedstock) (Ibarrola et al., 2012). LCA of most of the biochar exhibited by excessive biochar dosage in the AD process, and
applications brings positive impacts in comparison to conventional desirable biochar production conditions should be specified to
practices. GHGs emission was reduced to 2.74 kg CO2-eq kg1 make the biochar-amended AD process more productive and
biochar with the production from forestry waste, and its soil cost-effective.
application improved different impact categories such as human  Mechanisms of effective microbial metabolic routes in the
toxicity (HT), climate change (CC), freshwater eutrophication (FE), biochar-amended AD process are not completely understood,
and fossil depletion (FD) (Mun ~ oz et al., 2017). The integration of and more research efforts should be paid to biochar-microbe
pyrolysis of digestate and AD can elevate the net energy generation interactions and their effects in continuous-fed digesters.
with respect to AD alone (Monlau et al., 2015) and increase its soil  The roles of DIET and/or IIET encouraged by biochar require a
amendment quality (Monlau et al., 2016) with added environ- microcosmic and electron-based elucidation for maximizing
mental and economic advantages (Antoniou et al., 2019) (Fig. 6). CH4 production in the AD process and establishing a new avenue
Based on the LCA of biochar production and application, it is of research for up-gradation of the AD process and its products/
believed that biochar-amended AD can provide environmental by-products.
benefits in comparison to non-integrated processes (Li et al., 2018;  Biochar-amended co-digestion approach illustrates a positive
Righi et al., 2016). However, more LCA studies are required to synergy in reducing the design volume of reactors and pro-
establish relationships and quantify environmental contribution. ducing bioenergy from substantial amounts of food waste and
sludge simultaneously, but it also imposes new challenges due
to heterogeneity of waste compositions and reaction pathways/
7. Conclusions and prospects for future research thermodynamics, which deserve extensive investigation for
fostering technology commercialization and widespread
The properties and functionalities of biochar are significantly application.
dependent on the type of feedstock and pyrolysis process. Biochar  Techno-economic analysis in the pilot- and industrial-scale
has enormous prospective to be utilized in AD as an additive to studies together with material and energy balance assessment
elevate its productivity. The inclusive assessment of the latest are essential for the biochar-amended AD system. The
literature on the carbon-amended AD process revealed the application-oriented biochar production, optimized AD process,
conceivable priority of biochar in comparison to its counterparts and the associated energy consumption and biogas production,
such as carbon cloth, AC, graphene, maghemite/magnetite carbons etc., should be evaluated and justified from an overall life cycle
in view of the cost-effectiveness, simple synthesis process, and and supply chain management viewpoint.
improved biogas yield and digestate quality. In addition, magnetic  Sustainable and low-carbon management of solid and liquid
biochar is an iron-impregnated biochar composite with property of digestate generated after the process of AD is an important
magnetization, which can be recycled to reduce the costs of biochar issue. The application of the circular economy model for the AD
addition. Moreover, the recycling of magnetic biochar in the AD digestate management is necessary for closing the material flow
process may overcome the problem related to the loss of the loop. Solid digestate generated in the biochar-amended AD
methanogen population due to digestate disposal. Besides, Fe2O3 system can be further utilized in the fabrication of biochar for
and Fe3O4 impregnated biochar can act as electron conduits to subsequent recycling in the AD process or alternative applica-
encourage interspecies electron transfer. tions. Best practices of sustainable digestate management with a
It is noteworthy that the improved stability and reliability of AD circular economy model should be emphasized in future
with biochar reveals a novel paradigm to produce renewable en- investigations.
ergy, generate fertilizer-grade digestate, and minimize waste gen-
eration, presenting a more economical strategy for waste
biovalorization. Co-digestion of FW and sludge in biochar-amended
CRediT authorship contribution statement
AD system would be expected to demonstration beneficial syn-
ergies on reducing the digester volume and water footprint of the
Manish Kumar: Conceptualization, Methodology, Investigation,
AD process. It has been widely recognized that biochar can improve
Writing e original draft. Shanta Dutta: Investigation, Writing e
AD efficiency by mitigating the acidification impact caused by VFAs
review & editing, Validation, Visualization. Siming You: Writing e
accumulation, promoting electron transfer, providing adaptation to
review & editing, Validation. Gang Luo: Writing e review & editing,
high OLR, and supporting selective microbial growth. In compari-
Validation. Shicheng Zhang: Writing e review & editing, Valida-
son to GAC and traditional AD additives, an adequately designed
tion. Pau Loke Show: Writing e review & editing, Validation.
biochar additive can minimize potential environmental impacts
Ankush D. Sawarkar: Writing e review & editing, Validation. Lal
and maximize overall cost-effectiveness. Moreover, the integrated
Singh: Writing e review & editing, Validation. Daniel C.W. Tsang:
pyrolysis and AD system would be conducive to further improve-
Resources, Conceptualization, Supervision, Methodology, Investi-
ment in environmental performance and economic feasibility.
gation, Writing e review & editing, Project administration, Funding
Future studies are imperative to address the existing knowledge
acquisition.
gaps and limitations regarding biochar application as an additive in
the AD of FW and sludge, and the following research directions can
be proposed. Declaration of competing interest

 Biochar production and design with desirable properties by The authors declare that they have no known competing
science-informed methods and its possible synergy with vari- financial interests or personal relationships that could have
able additives warrant extensive investigation. appeared to influence the work reported in this paper.
18
M. Kumar, S. Dutta, S. You et al. Journal of Cleaner Production 305 (2021) 127143

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