Biomass and Bioenergy 186 (2024) 107271

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Biomass and Bioenergy

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

From raw material powder to solid fuel pellet: A state-of-the-art review of

biomass densification
Haomeng He , Yu Wang , Yu Sun , Wanfeng Sun , Kai Wu *
School of Mechanical Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China

A R T I C L E I N F O A B S T R A C T

Keywords: Densification is the most effective forming technology, the production of which, pellets are the most intensive
Densification energy content of biomass solid fuels. Increasing the overall utilization efficiency of bioenergy, extending
Biomass feedstocks available types of wastes and residues for pelleting, and improving the pellet quality comprehensively are
Pelleting process
necessary. This paper reviewed feedstocks used for pelleting, binding mechanism of biomass pellets, and eval­
Pellet quality
Binding mechanism
uation systems of pellet qualities. To extend the supply amounts and improve the qualities of raw biomass,
various feedstocks and formulation recipes were classified based on their regions, sources, and species. And
applicable objects and conditions of several different pretreatment technologies for feedstocks were compared.
Physical properties and biochemical analyses are also concluded to evaluate the flowability, compactibility, and
potential characteristics as solid fuel. For a better understanding of energy consumption and conversion during
the densification process, pelleting devices and binding mechanism are elaborated. Associations and differences
between single pelleting press in lab-scale and industrial pelleting in pilot-scale are also discussed. Suggestions
are proposed for the optimization design of pelleting devices and processes for different feedstock densification.
Lastly, relationships between operating parameter factors of pelleting process and pellet quality are presented.
This review could provide theoretical analyses for powder compression, new insights for waste to energy, and
guidance for achieving global peak carbon and environmental strategic objectives.

enchanted with higher heating values, better grindability, and higher

1. Introduction water resistance [10].
Pelleting and briquetting are common industrial densification
With the implementation of the global peak carbon policy, bioenergy manufacturing processes. However, higher energy consumption, wear,
is paid more attention once again because of its ability to zero or and deformation of key components (roller and die) of the pelleting
negative carbon emissions and carbon capture and storage [1,2]. devices in industrial pelleting have been the major unsolved problems
Biomass is abundant and potential renewable energy all over the world [11]. Currently, with the biomass feedstocks appearing continuously,
not only in amounts but also in species [3,4]. The utilization of biomass the suitability and robustness of the pelleting devices remain to be
energy is also in line with the concept of waste to energy to solve solved, and it may even need a dedicated roller and die design for the
environmental pollution and landfilling management issues [5]. So, it is densification of some feedstocks. Furthermore, the conversion mecha­
necessary to explore and expand the potential of biomass. However, nisms of energy consumption during the densification process are still
biomass with intrinsic defects such as low energy content and high not clear, specifically the actual energy used for compression, extra
operational costs for their management, collection, transportation, and energy wastes due to heat generated by friction, and losses of pellets by
storage was not popular [6]. Densification was an effective method to excluding from the mechanical devices [12,13]. Increasing the propor­
solve it, which means loose biomass powder converting into shaped and tion of actual energy consumption enhances the efficiency of the ma­
formed solid fuel under pressure in a certain volume [7,8]. Moreover, chine. Appropriate energy consumption helps the binding of biomass
biomass materials have several disadvantages: hydrophilic properties, pellets, too high reduces mechanical equipment life expectancy, and too
higher moisture, lower heating value, and heterogeneous properties [9]. low forms inferior pellets.
Several pretreatment technologies coupled with densification are arising Traditional resources of biomass pellets mainly are from local in­
to improve these shortcomings, biomass after pretreatments will be dustrial sawmill residues, this supply chain is very easy to break down in

* Corresponding author.
E-mail address: [email protected] (K. Wu).

https://doi.org/10.1016/j.biombioe.2024.107271
Received 17 April 2024; Received in revised form 23 May 2024; Accepted 27 May 2024
Available online 31 May 2024
0961-9534/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
H. He et al. Biomass and Bioenergy 186 (2024) 107271

Nomenclatures UV-A Ultrasonic-vibration assisted

LM Light microscopy
MSW Municipal solid waste SEM Scanning electron microscopy
RDF Refuse-derived fuel CT Computed tomography
LDPE Low-density polyethylene L/HHV Lower/High heating values
PP Polypropylene TEA Techno-economic analysis
AOR Angle of response LCA Life cycle assessment
HR Hausner ratio GHG Greenhouse gas
CI Carr-index
C, H, O, N Carbon, hydrogen, oxygen and nitrogen Symbols
CMC Carboxymethyl cellulose Tg Glass transition temperature
HTC Hydrothermal carbonization R2 R-square
LHW Liquid hot water SO2 Sulfur dioxide
SE Steam explosion NOx Nitrogen oxide

a region and makes feedstock storage inadequate [14,15]. The amounts guarantee the supply chain and quality of biomass feedstocks, various
of biomass feedstocks should be guaranteed the market supply, feed­ biomass feedstocks used for pelleting are classified and reviewed in
stock types are also the limitation factors of pellet qualities. So, it is Section 2; to optimism the pelleting process (reducing extra energy
necessary to expand multiple resources of biomass feedstocks, which not consumption for pelleting and optimizing pelleting processing), how
only guarantee the supply chains but also improve the pellet qualities to biomass powder converting into pellet were discussed in Section 3; to
meet demands for industrial uses. In addition, extending the use of en­ evaluate pellet quality comprehensively, factors affecting pelleting
ergy crops and non-food can avoid competition with human food and process and pellet quality are reviewed in Section 4; finally, some
animal feed as well as reduce the effects on food prices [3,5]. Pellets emerging conceptions used for industrial pellet production are discussed
from single component feedstock cannot meet the requirements of the in Section 5.
market, exploring multiple component and pellet formulation of
biomass feedstocks is also a hot topic [16]. 2. Biomass feedstocks
In summary, biomass feedstocks should be used for local supply re­
quirements based on the region and avoid long-distance transportation With listed targets as shown in Fig. 1, physical properties and
and logistics as much as possible. However, from the perspective of biochemical components of feedstocks, type classifications and formu­
supply and demand, biomass energy in North Europe is huge but lation recipes used for pelleting, and several pretreatment technologies
available bioenergy resources may be insufficient, while Southeast Asia of feedstocks are reviewed in this section.
is the opposite. Therefore, research about market supply, logistics costs,
and biomass pellet quality is proposed to satisfy and balance the growing 2.1. Physical properties
global energy demand [17]. Once involving traveling long distances and
time storage across oceans, several indicators of pellet qualities should Physical properties of biomass particles can evaluate the potential of
be improved, especially for microbial biodegradation, mechanical feedstock to be pelleted and are necessary for theory modeling analysis
durability, and water sorption. In this case, mechanical strength, hy­ and computer simulation [43]. Some basic physical properties mainly
drophobicity, and energy content of biomass pellets need to be enhanced include particle size distribution, moisture content, particle shape, true,
[18,19]. bulk, and tapped densities, and there are comprehensive standards to
Biomass pellets are also precursors for thermochemical and measure and calculate [44]. Hausner ratio (HR) and Carr-index (CI) are
biochemical conversions such as combustion, gasification, pyrolysis, calculated by bulk and tapped densities, which were used to assess
and biorefining [20–23]. Therefore, some studies have been carried out compressibility and compactbility, while the angle of repose (AOR) re­
based on these, such as the sugar yield of raw materials and biomass flects the flowability of feedstocks [43]. Rezaei [45,46] observed
pellets [22]. Biomass pellets also have potential applications in energy biomass particles with the microscope and calculated the shape factors
production [24,25], combined heat and power [15,26], iron and steel (width, length, aspect ratio, sphericity, circularity, and roundness) of a
industry (the pulverized coal can be replaced by bio-char from pyrolysis single particle through image processing. Guo [47] measured the par­
and torrefied biomass [27–29]), and residential or commercial heating ticle shape and particle size distribution characteristics of different
[30,31]. biomass feedstocks. Kang [38] presented detailed definitions of powder
Up to now, biomass densification technology has developed into densities and compared them for different purposes. The obtained re­
some stages, there were already several reviews in the past decade. sults indicate biomass particle shape and particle size distribution were
Nielsen [11] and Stelte [32] summarized the mechanical structures and mainly determined by milling methods and conditions and influenced
parameters of the roller and die. Kaliyan [33], Whittaker [34], Mostafa on densification process. The bulk density of particles depends on par­
[35], Cabral [36], and Gilvari [37] discussed the affecting factors and ticle size, the smaller the particle sizes the higher the tapped density [48,
their effects on pellet qualities. Kang [38] and Sarker [39] elaborated 49]. Most biomass particles have poorer flowability properties, which
the binding mechanism during the densification process. Sithole [40], may block feeding system in the pelleting process [50,51]. There is a
Yu [41], and Eling [42] explored the effects of co-pelleting of pre­ reduction in the particle length during pelleting, which results in higher
treatments and densification on pellet qualities. All these reviews only particle circularity and elongation (width-to-length) ratio values, and
reported the densification technologies partly, and new industrial future the pelleting process alters the shape and length of particles [52].
trends are also not captured. Therefore, based on the series of afore­
mentioned and summarized questions as well as existing reviews, a 2.2. Biochemical analysis
comprehensive discussion on biomass densification from three aspects:
biomass feedstocks, pelleting process, and pellet quality is presented. Kaliyan [33] and Arshadi [53] explained the effects of different
And detailed structures of this review are organized as follows: to constitute (starch, protein, fiber, and fat) of feed pellets on the binding

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H. He et al. Biomass and Bioenergy 186 (2024) 107271

Fig. 1. Organization framework to analyze and classify the biomass feedstocks.

mechanism, the essence transforms powder into pellet is the compre­ biomass densification. And it is very necessary for an emerging material,
hensive effects of heat, moisture, compressive stress, friction force and the feedstock was first subjected to comprehensive analyses of physical,
mechanical shearing on biomass feedstock during the densification chemical, thermal, and fuel properties.
process, and argued the binding mechanism of feed ingredients can be
extended from the known to the unexplored similar with from feed to 2.3. Biomass feedstocks used for pelleting
biomass densification. Compared with components of feed, there were
more cellulose, hemicellulose, lignin, and extractives for biomass feed­ Biofuels are classified into first, second, third, and fourth generations
stocks. Lignin softening, flowing, and hardening, protein denaturation based on their origins, sources, types of raw material, and conversion
and plasticization, as well as starch gelatinization result in solid bridge processes [3], and their characteristics, limitations, and advantages are
binding into biomass pellet during the pelleting process [54,55]. Lignin also discussed in detail by Babu [5] and Yong [75]. Moreover, different
with its self-bonding behavior can serve as a natural binder if used as an types used for biofuel production were defined as biomasses (wood,
additive to make stronger and more durable pellets for energy and other herb, agriculture, forestry, and aquatic) and wastes (animal and human,
biorefinery applications [56]. Waxes and fats present in the extractives contaminated biomass, and industry wastes) [10,76].
have dual effects, diminishing the friction in the die channels and pre­ Single and multiple components: based on the number of feed­
venting the formation of strong bonds through the formation of a weak stock types used for pelleting, biomass feedstocks can also be defined as
boundary layer among the particles [57,58]. The binding mechanism of single and multiple components. There is only single pure biomass
cellulose and hemicellulose in the pelleting process is not studied feedstock for pelleting in single component, and traditional single
equally the same as lignin and extractives. component mainly includes sawdust [15,77,78], poplar [79], peanut
For biomass feedstocks in pyrolysis, proximate and ultimate analyses shell [80], grasses [81], corn stalk and its residue [82,83]. Recently
were measured to evaluate whether to meet the demand for biofuel [59]. more diverse feedstocks were pelleted such as onopordum [84], melon
Considering the pelleting process and pellet qualities have relationships stalks [85], hazelnut shells [14], elephant dung [86], and coffee grounds
with chemical component contents, this may help understand the pel­ [87,88]. Researchers also try several different feedstocks for pelleting,
leting mechanism quantitatively. There are several comprehensive re­ which could be called multiple components, to compare their pellet
views about ultimate analysis (C H N O and other chemical elements) quality and potential such as Cui [55] (apple tree branches, corn cobs,
[60,61], proximate analysis (fixed carbon, volatile matter, ash, and sunflower seed husks, and microalgae), Siyal [89] (furfural residue,
moisture) [62], and heating values [63] for common biomass feedstocks. sawdust, corn stalk, and sewage sludge), San [90] (four woody and three
Toscano [59], Biswas [64], and Singh [65] reported proximate and ul­ herbaceous), Agar [91] (eight woody), Frodeson [92] (twenty-one
timate analyses when biomass pyrolysis. Several papers have published different feedstocks), Christoforou [93] (eight agricultural and indus­
chemical components of various biomass [5,66–69]. Ultimate and trial), and García [94] (twelve lignocellulosic). Blends and mixtures of
proximate analyses were used to evaluate pellet fuel characteristics, non-edible energy crops and their by-products (industrial processing
while chemical components could be used to analyze the densification waste) are also used for pelleting, such as torrefied pine with solid and
process and pellet quality. For further studies, comprehensive in­ liquid residues [95], onopordum and its seed oil [84], and oliver stem
vestigations about chemical components, proximate and ultimate ana­ with pyrolysis oil [96].
lyses of biomass feedstocks should be conducted to establish databases Regional and seasonal biomass: published papers also evaluated
about biomass characteristics such as references [63,70–74] before the developed potential of feedstocks to be pelleted in cases from the

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H. He et al. Biomass and Bioenergy 186 (2024) 107271

point view of regions (China [97], Philippines [98], Mexico [99], Greece primary feedstock. Based on the proposed method [38], several empir­
[100], Zambia [101], and other countries [102,103]), seasons (peren­ ical studies about slight additions of additives were discussed below in
nial industrial crop biomass [104,105], and short rotation woody crops Table 1.
and forest biomass [106]). Nguyen [18] also reported the effects of The varieties and amounts of additives used for pelleting are abun­
vigorous and moribund trees on pellet qualities. dant in the lab-scale, while there are strict standard limitations for the
Municipal solid waste: with the target of waste to energy, energy amounts of additives in the industrial scale for environmental safety.
generation from non-hazardous wastes is also proposed [107]. The Therefore, researchers have tried to use two or more types of materials
combustible fraction of municipal solid waste (MSW) was termed (multiple components) for co-pelleting to overcome those shortcomings
“Refuse-derived fuel (RDF)”. García [108] studied the co-pelleting of (insufficient supply of regional biomass; lower compressive strength and
RDF and pine sawdust in a continuous pilot pelleting press. Blending energy content of pellets; higher ash content) of single component.
paper, organics, and wood as typical RDF for pelleting to investigate the Several biomass feedstocks and industrial wastes act as natural binders
pellet qualities was conducted [109]. Marais [110] used coal fines as or additives such as orange peels rich with pectin and tubers rich with
primary materials with low-density polyethylene (LDPE) and poly­ starch to improve pellet quality and bamboo rich with lignin to enhance
propylene (PP) as additives to pellets. Emadi [111] combined herba­ energy content. To improve the high content of ashes and low energy
ceous biomass and LDPE for pelleting and proved ash content of biomass content of rice straw pellets, different proportions of bamboo were
pellets decreased with the increase of LDPE. Nasiri [112] evaluated the added to rice straw to investigate the effect of mixing ratio on the pellet
solid waste from various sections of the compost residue to be pelleted. properties [127]. Moreover, the uniformity of feedstock blends should
LDPE and PP were used as binders for the briquetting of sawdust [113]. be focused on because of their physical properties such as poor flow­
Sewage sludge is a by-product from municipal wastewater treatment ability, Cheng [141] mixed biomass feedstocks with coal tar residue by
plants, which contains significant amounts of organic compounds thermostatically water bath. There were studies about the various for­
(mainly proteins and carbohydrates) [114,115]. The denaturation of mulations and mixing ratios of feedstocks to conclude as below in
protein and the gelatinization of carbohydrates in the sludge could serve Table 2.
as natural binders to improve the strength of the fiber grid in pellets There were two or more kinds of materials for a multiple component
[116]. There were several studies to conduct on the functions of process in Section 2.3. According to their function for pelleting, they can be also
parameters for sewage sludge and biomass pelleting [54,89,117–119]. defined as binders, additives, and lubricants. All those have dual effects
Co-firing biomass with coal: Coal and biomass co-gasification with on pellet quality, and positive effects on pelleting process, especially for
carbon capture and storage is regarded as a promising cost-efficient biomass after pretreatment and biochar. More and more binders were
option to mitigate greenhouse gas (GHG) [120,121]. Published used to strengthen the binding mechanism of biomass pellets; and ad­
research of co-firing, co-pyrolysis, and co-gasification between biomass ditives can be used as emissions alleviators, and combustion condi­
and coal released a basic theory to conduce industrial co-pelleting tioners to increase fuel qualities, combustion performance, and thermal
hopefully [122–124]. Lu [125] reported a crop residue ratio of 35 % conversion process; while lubricants were used to improve the pelleting
could produce electricity with net-zero life-cycle GHG emissions. Based process. And friction loss between die wall and feedstocks may be
on all the above reported conclusions and considering the environment reduced with the existence of additives and lubricants, while increased
and economics, there is an increasing tendency to co-pelleting for because of binders [38,144]. Proper friction helps generate heat for
biomass and coal. binding, too much for blockage, too little may decrease the compressive
strength [11]. There are discussions about the effects of common binders
2.4. Biomass blends and mixtures used for pelleting. Kong [145] investigated the effect of one binder and
four hardeners on properties of biochar pellets, binders cause moisture
Different biomass feedstocks have their specific properties, and it is uptake to disrupt mechanical properties of biochar pellets, while hard­
hard for single component material to meet demanded pellet quality in eners may reduce the moisture uptake on reducing the disruptive force
some situations. Eisenbies [126] proposed blending is combining com­ and play the effects of hardening and water resistant. Muazu [146]
plementary materials for pelleting to enhance comprehensive pellet studied the effects of starch, biosolids, and microalgae on density,
quality grade, and distinguished the definition of blended, aggregated, durability, energy content, and combustion characteristics of fuel bri­
and amended feedstocks. ISO 17225-7 defined blends are intentional quettes. Results show microalgae had positive effects on density and
mixed biofuels, while mixtures are unintentional, which can be also strength; biosolids improved pellet density, but had a negative effect on
explained: blends refer to feedstock proportions are mainly determined strength; starch enabled compressive strengths, but significantly
by manual operation, while mixtures refer to feedstock distribution are reduced density. Si [147] used additive solution (carboxymethyl cellu­
in the natural state. Cui [14] also concluded mixing different biomass lose, CMC) to investigate influence of binder on physical and mechanical
feedstocks for co-pelleting is a promising way to upgrade pellet quality properties of agricultural stalk pellets. Pellet quality exhibited a signif­
and facilitate pelleting process. Taking examples of animal feed, feed­ icant increase, while energy consumption was decreased with the in­
stock formulation recipes were developed [33]. The purpose of formu­ crease of CMC content. CMC is an effective binder for biomass with
lation recipes is to pair poor-performing feedstocks with lower extractive content. Wang [148] studied four municipal solid
high-performing feedstocks with one or more components to make a wastes (dog manure, horse manure, apple pomace waste and tea waste)
greater range of feedstocks available and produce more uniform pellets with an industrial by-product to produce solid fuel pellets. The
[126]. by-product showed the feasibility for the production of solid fuels.
According to the relative weight content ratio of biomass feedstocks Behjoee [149] used sodium lignosulfonate as an additional binder to
for pelleting, Kang [38] also defined those materials into primary improve pellet density, tensile strength, impact resistance, and water
feedstocks, secondary feedstocks, and additives. The primary feedstock uptake capacity. Mediavilla [79] concluded starch and lignosulphonate
refers to the main constituent of the pellets. The secondary feedstock is both increased the pelleting process stability and decreased the specific
added to the pellet with a content lower than the primary feedstock but energy demand, while starch had better performance at the same
significantly higher than additives. And it is mostly generated from dosage. Wang [150] also investigated the effect of four organic binders
biomass conversion or other waste treatments or processes. The addi­ (protein, starch, lignin, and molasses) on woody biomass pellets. Results
tives refer to the materials added to the pellets with the smallest showed pellets with starch and protein have better tensile strength than
amounts (usually <20 % in lab research [38]). Another problem needs those with lignin and molasses, considering protein has higher cost,
to be considered is the costs, the price of the secondary feedstock is starch as binder is preferable. Ningsih [151] identified the effects of pine
typically lower than that of the additives but higher than that of the sap as additive on the longest flame of pine flower briquette. Yang [56]

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Table 1
Summary of selected studies for biomass blends and mixtures.
Primary feedstocks Secondary feedstocks Binders, additives and Mixing ratio (%) Ref.
lubricants

rice straw bamboo – 100:0; 80:20; 60:40; 40:60; [127]

20:80; 0:100
rice straw pine sawdust – 0; 20; 40 [128]
sodium lignosulfonate 0; 10; 20
sugarcane bagasse rice bran – 100:0; 80:20; 60:40; 40:60; [129]
20:80; 0:100
walnut shells cones – 100:0; 75:25; 50:50; 25:75; [130]
0:100
sewage sludge furfural residue – 100:0; 80:20; 60:40; 40:60; [119]
corn stalk 20:80; 0:100
coal slack wheat bran – 4; 10; 20 [131]
sawdust wheat straw – 100:0; 80:20; 60:40; 40:60; [132]
rapeseed straw 20:80; 0:100
date seeds coconut shell – 50:50 [133]
microalgae biochar 30:70
30:40:30
polyalthia longifolia leaves wild taro tubers – 10; 15; 20 [134]
bamboo charcoal 0; 25; 50
pine sawdust coffee dregs/coffee husks/cocoa shells/grape pomace – 90:10 [94]
almond shells/miscanthus/olive stones/pine cone leaves/pine – 85:15
kernel shells/hazelnut shells
grape pomace – 80:20
almond shells/miscanthus/olive stones/pine cone leaves/pine – 70:30
kernel shells
A4 papers paraffin wax – 100:0; 90:10; 80:20; 70:30; [135]
60:40; 50:50
wheat straw – calcium carbonate 2; 6; 10
cassava starch [136,
137]
fallen leaves – glycerol 0; 5; 10 [138]
sugarcane bagasse lignocellulosic cake – 100:0; 75:25; 50:50; 25:75; [139]
0:100
– glycerol 0; 1; 2; 3
torrefied pine – glycerol [95]

4; 12; 16; 18; 20; 30

grape pomace 10; 20 /0, 10, 20, 30
25; 50; 75 /0; 10; 20; 30
pine
sawdust ground nut shell – 20; 40; 60 [140]
leaf litter waste
ground nut shell sawdust
leaf litter waste
leaf litter waste sawdust
ground nut shell
sawdust/ground nut shell/leaf – recovered polyvinyl 2; 4; 6
litter waste alcohol
waste cooking oil
waste lubricating oil

Note: “/” in the table means parallel combinations, such as pine sawdust: coffee dregs/coffee husks refer pine sawdust: coffee dregs and pine sawdust: coffee husks
respectively.

utilized corn stover as feedstocks and its hydrolysis residue as additives industrial transport standards, while on the other hand, removing or
to improve combustion performance, short process time, and enhance changing the definition of durability indicator because it could not
water penetrations and droplet absorptions. Sarker [152] reported completely reflect real applied force on pellets, the issue will be dis­
mustard meal, lignin, and bio-oil as binders can increase the density, cussed in Section 4.1. In this subsection, biomass feedstocks were dis­
durability, and tensile strength of canola residue pellets by 21 %, 20 %, cussed based on their function (binders, additives, and lubricants) and
and 123 %, respectively. formulation recipes, respectively.
Above all, biomass blends and mixtures for pelleting are practicable.
Exploring new biomass feedstocks for pelleting with the target of spe­ 2.5. Biomass pretreatment technologies
cifically improving pellet quality: shells for enhancing energy content
and peel for strengthening durability. The types and amounts for addi­ To some extent, the densification process also belongs to pretreat­
tions need more elaborate examinations to make this strategy com­ ment technology and physical as well as mechanical conversion of
mercial and industrial in the future under the guidance of environmental biomass, and it is out of the scope in this section. There were some
safety. These studies also explained the role of different chemical com­ available review papers on the effects of several pretreatment technol­
ponents during densification process from the point of pellet quality. ogies on the pelleting process [8] and the advantages and disadvantages
The most evident behavior for pellets is density increases, while energy of various pretreatment technologies [10]. Yu [41] reported biomass
consumption and durability decrease. The former two are desired, while feedstocks become more homogeneous and higher binding ability after
the latter one is controversial. On the one hand, the decreased durability the pretreatment process. Improving the physical properties of feed­
can be accepted as long as the indicator meets the requirements of stocks to contribute pelleting process and pellet quality, and enhancing

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H. He et al. Biomass and Bioenergy 186 (2024) 107271

Table 2 purpose of torrefaction is to remove moisture and some volatile organic

Formulation recipes of biomass feedstocks. matter, while the final products of pyrolysis are liquid (bio-oil), gas
Template format: feedstocks spices (proportion/%) Ref. (hydrogen, methane, and volatile matters), and solid (biochar). Torre­
faction and pyrolysis usually were preferable for dry biomass feedstocks.
coffee grounds (100) [87]
coffee grounds (25), rapeseed straw (75) Specific discussions were reviewed based on the sequential processing
coffee grounds (50), rapeseed straw (50) steps of pyrolysis, torrefaction, and pelleting in this subsection.
rapeseed straw (100)
chaff (100) (1) Pyrolysis before pelleting
coffee grounds (50), chaff (50)
dry leaves (100) [142]
rice husk (100) Kong [145] investigated the effect of one binder and four hardeners
dry leaves (60), rice husk (20), sawdust (20) on the conversion of biomass into bio-char pellets at the temperature
rice husk (60), dry leaves (20), sawdust (20) range of 200–700 ◦ C and proved most volatiles in biomass decomposed
sawdust (40), dry leaves (30), rice husk (30)
at 200–300 ◦ C during the pyrolysis process. Hu [160,161] elaborated a
sawdust (50), rice husk (50)
wheat straw (100) [143] deeper understanding of biochar binding mechanism and investigated
wheat straw (80), sawdust (10), bentonite clay (10) the effects of different binders (lignin, starch, calcium hydroxide, and
wheat straw (80), sawdust (10), corn starch (10) sodium hydroxide) on the properties of biochar pellets which were
wheat straw (70), sawdust (10), bentonite clay (10), glycerol (10) pre-treated with temperatures from 250 to 650 ◦ C. Kang [96,162] con­
wheat straw (70), sawdust (10), bentonite clay (10), biochar (10)
wheat straw (70), sawdust (10), corn starch (10), biochar (10)
ducted pelleting experiments with biochar and bio-oil, with pyrolysis
wheat straw (60), sawdust (10), corn starch (10), bentonite clay (10), temperature is 500 ◦ C for 60 min. Riva [163] proposed a method to
biochar (10) produce biochar: pyrolysis at 600 ◦ C, densification with pyrolysis oil as
grass mowing residues (100) [13] binder, reheating obtained pellet, and optimizing the processing pa­
palm pruning residues (100)
rameters. Gul [28] applied the new methods to produce biochar by
agricultural residues (100)
mix1: 50 % agricultural residues + 50 % (spruce + eucalyptus + acaia) pelleting charcoal with pyrolysis oils and reheating it at high tempera­
pruning residues tures to obtain materials with sufficient hardness and proper reactivity
mix2: 50 % grass mowing residues+50 % mix 1 for metallurgical coke. It also gives a new method to expand the shaped
mix3: 50 % palm pruning residues+50 % mix 1 biochar pellets in steel industry. There was also report about palm kernel
shell residues from the gasification were compacted into solid fuel bri­
the energy content of unit mass for feedstock are the main purposes of quettes [164].
pretreatments [21]. Life cycle assessment indicated more energy input
enhanced energy return ratio for co-pelleting with pretreatment and (2) Torrefaction before pelleting
densification. Pretreatment technologies are conducive to modifying the
heterogeneity of biomass feedstock, increasing the adaptability of Sarker [152] studied the relationship between microwave torre­
biomass feedstock during pelleting, reducing contents of NOx and SO2, faction power, time and feed loading rate, relaxed density, durability,
and improving thermodynamic quality of pellets [153]. and strength of pellets. Chen [165] investigated torrefaction tempera­
tures 200, 250, and 300 ◦ C for 30min and explored the bonding mech­
2.5.1. Products of pretreatment anism of in-situ torrefied densified pellets. Cao [166] pre-treated
Biochar is the most solid product of pretreatment technologies. Thus, biomass at different torrefaction temperatures (240, 270, and 300 ◦ C) to
most studies have been conducted and focused on how biomass feed­ reveal the complementary mechanisms between torrefaction and
stocks were treated under different pretreatment technologies and co-pelleting for biomass pellet preparation. Bai [167] measured physi­
experimental conditions to obtain biochar as well as its densification. cochemical and friction characteristics of raw biochar and reported
Biochar is carbon-rich microporous material and has the potential for pellets from torrefaction temperature of 275–300 ◦ C have best qualities.
agriculture, environment, and energy as biochar-based fertilizer, cata­ Yang [168] conducted effects of torrefaction temperature (280 and
lyst support, and carbonized bio-coal, respectively [154–156]. Chen 300 ◦ C), hold time of compression (6 and 10 min), pressure of densifi­
[157] has tried to replace fossil fuels with biochar (carbonized bio-coal) cation, moisture content of torrefied biomass on the durability and hu­
in China’s rural energy upgrading progress and pointed out compressed midity resistance of pellets and obtained optimal condition parameters.
and shaped biochar with superior combustion properties, which pro­ Though biomass after pyrolysis has better homogeneous performance,
vided a new method for biomass to combine pretreatment technologies pyrolysis made biomass feedstock more unable to pellet and these usu­
with densification for co-pelleting. Biochar has higher coefficient of ally need to be improved the help of binders for pelleting [152].
friction and lower cohesion than raw materials, those characteristics
change with pretreatment parameters, which also means less potential (3) Torrefaction after pelleting
to be pelleted. Therefore, published papers about pretreatment tech­
nologies and biochar densification usually appear with binder additions. Manouchehrinejad [169] investigated effects of torrefaction at
Besides, Behjoee [149] used canola meal and oat hull as raw materials to temperature ranges 230–290 ◦ C for 30 min on the physical quality and
produce biosorbents, water uptake capacity of those pellets could be fuel properties of torrefied pellets and obtained energy-dense pellets in
comparable or higher to commercial adsorbents. the range of 275–280 ◦ C. Siyal [170] studied the influence of torre­
faction process variables (temperature 200, 250, and 300 ◦ C and resi­
2.5.2. Torrefaction and pyrolysis dence time 15, 30, 45, 60 and 120 min) on pellet quality parameters and
Torrefaction and pyrolysis are common thermochemical conversion proved torrefaction after pelleting improved heating value and resis­
pretreatment technologies to improve the physical and chemical prop­ tance to water uptake. Wang [171] conducted the torrefaction temper­
erties of biomass, which are conducted at the temperature range of ature (225 and 275 ◦ C) for 30 and 60 min respectively, and reported
200–1000 ◦ C in an oxygen-free or inert atmosphere [6,158,159]. Kota energy for grinding torrefied pellets reduced by 50 % and narrower
[158] presented comprehensive views of torrefaction mechanism. particle size distribution. Zhang [172] conducted torrefaction temper­
Escalante [159] explained the basic reaction mechanism of pyrolysis. ature from 200 ◦ C to 350 ◦ C for 45 min and reported torrefied pellets
Processing temperature and duration time of both torrefaction and py­ with higher hydrophobicity than raw pellets, furthermore with torre­
rolysis are different, torrefaction is a milder process than pyrolysis. The faction temperature arising, cracks on the surface of torrefied pellets
increase and mechanical properties reduce. Jezerska [87] evaluated

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torrefaction process on the physical, mechanical, and energy properties for pelleting is increasing [188,189]. Biomass feedstocks will be more
of pellets. Torrefaction had positive effect on the energy parameters C/O fine and brittle after SE pretreatment with SO2 as catalyst, and lignin
and C/H ratio, fixed carbon and LHV increase, no significant impact on was probably sulfonated to lignosulfonates as lubricant with the SO2
the ash melting point while negative effect on increasing the ash, N, and catalysing to reduce energy consumption [41]. Whereas researchers put
S content. However, Agar [173] argued torrefied pellet production more attention on enzyme-mediated bioconversion during the pre­
cannot compete economically with conventional production from the treatment but seldom on pelleting. One more question need to be solved
point of production costs. is that the total cost and energy consumption of SE process is higher than
pelleting and it is not economic. And it also was not promoted in in­
2.5.3. Hydrothermal carbonization (HTC) dustrial pilot, both require further study and attention.
HTC pretreatments can modify the complex structure of hemicellu­
lose, cellulose, and lignin; dehydration, decarboxylation, and aromati­ 2.5.6. Other technologies
zation reactions occur during the process, both of which are good for Besides the above-mentioned mainstream pretreatment technolo­
making durable pellets [174]. HTC pellets are expected for high com­ gies, researchers are also exploring other technologies for biomass.
bustion efficiency and low pollutant emissions. Because of high adapt­ Zhang [190] investigated effects of different pretreatments (natural air
ability to wet biomass, municipal solid waste and industrial residues drying, vacuum sealing, 4 % ammonium hydroxide and vacuum sealing)
with high moisture contents (agricultural digestate, sewage sludge, and on characteristics of compression properties and energy consumption.
microalgae) are preferable pre-treating for these methods [175,176]. Liu Results showed pretreatments affected the forming and combustion
[177] reported some mechanical, storage, and combustion properties of characteristics, hemicellulose content had the positive correlation with
pellets (fixed carbon, heating values, energy contents, combustion energy consumption while lignin level had the negative correlation with
temperature range, and tensile strength) after HTC treatments combustion characteristic. Huang [191] proved the hemicellulose con­
increased, while the others (length expansion, moisture uptake, tent was decreased, while lignin content was gradually increased after
maximum weight loss rates, and residues) decreased. Though in recent 34-days anoxic storage. Then HHV and density of pellets were
studies types of biomass feedstocks and the preparing operating condi­ decreased, but the fixed carbon, ash content, compaction and extrusion
tions (temperature and residence time) are different during the HTC, energy consumption were increased. And results showed anoxic storage
similar scientific results and variate tendencies are obtained by Refs. could be against to enhance pelleting.
[175,178–180]. For fully utilizing the productions of HTC with pellet­
ing, Seraj [179] introduced HTC aqueous phase as a source of moisture
in pellet formulation. Yu has finished a series of scientific research about 2.6. Summary
HTC pretreatment technologies under different pretreatment operating
parameters [174,181–183]. Krysanova [184] verified HTC has greater This section is mainly reviewed relative to current research about
carbonification effect of biomass than torrefaction, which is expressed in biomass feedstocks and the main conclusions are summarized as follows.
greater transformation of the structural components and greater
modification. (1) Physical and biochemical characteristics of emerging biomass
feedstocks before pelleting are essential to optimize pelleting
2.5.4. Liquid hot water (LHW) process and assess pellet quality.
The purpose of LHW is to adjust contents of hemicellulose and lignin (2) Biomass feedstocks should be classified into primary feedstocks,
and ultrastructure of the cell wall to make biomass into soluble parts. secondary feedstocks and additives (binders and lubricants) and
Chen reviewed the reaction mechanism, reactor characteristics, and built a feedstock information database based on relative contents
influencing factors of LHW in biomass pretreatment [66]. LHW pre­ of chemical component or other advanced analytical methods
treatment involves moderate temperature (140–180 ◦ C) and extended (Fourier transform infrared spectroscopy and Raman spectrum)
period (30–180 min). Comparing with torrefaction, LHW treatment is to better predict pelleting process and pellet quality.
less energy-extensive drying process. Biomass feedstocks after HWT (3) The assessment of each potential value chain for emerging
process have higher energy content, higher dimensional stability, higher biomass feedstock requires knowledge of involved processing and
compressibility and lower spring-back, higher resistance to biodegra­ verification by numerous experiments. This explains why many
dation and lower pollutant emissions during combustion [18]. Eisenbies studies recently are conducted based on types of biomass feed­
[126] proved short rotation woody crops after LHW have better pellet stocks or formulation recipes.
quality grades than the untreated. Sermyagina [185] reported the (4) The essence of pretreatments is the variations of relative contents
combustion behavior was negligibly affected, volatiles and fixed carbon of chemical components (cellulose, hemicellulose, and lignin) to
of LHW pellets were only slight decrease in reactivity comparing with have effects on pelleting process and pellet quality. Torrefaction
untreated pellets. Though LHW is a promising biochemical conversion and pyrolysis are preferable for dry biomass, while HTC, LHW
for biomass into biofuels, there were some difficulties in optimizing and SE use water as medium for wet. And most torrefaction
reaction conditions. temperature usually ranges from 250 to 300 ◦ C, pyrolysis has
higher temperature but no more than 700 ◦ C. Processing condi­
2.5.5. Steam explosion (SE) tions of LHW and SE technologies are stricter to achieve or
Yu [41] reviewed the reaction mechanism, operating condition and extend.
parameters of SE and summarized the effects of SE on the pelleting (5) Densification and pretreatment technologies have separate ben­
process and pellet quality. The reaction mechanism is similar with HTC: efits on improving biomass pellets, the combination of densifi­
lignocellulosic matrix is broken down; hemicellulose is removed; lignin cation and pretreatment will be promising and dominating co-
is partially removed or redistributed during the SE process and cellulose pelleting process for solid fuel pellets in the future. By contrast,
accessibility is significantly improved after SE pretreatment [186,187]. torrefaction has been considered promising technique for
The variations of chemical component may cause particle size reducing biomass feedstock to produce high energy density, hydropho­
and lignin redistributing, and that is explaining why more robust bicity and uniform-quality biomass pellets.
binding mechanism among the particles after SE occurs when pelleting. (6) Emerging feedstock can be pre-treated and refined in energy and
Previous studies have reported SE modify enzymatic conversion and chemistry industry. The productions of pretreatment such as
pellet durability, and some production contents after biomass SE pre­ (biochar and bio-oil) are promising and potential raw materials
treatment arise which has positive with HHV, while energy consumption and provide new processing for pelleting.

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3. Pelleting process depending on their pelleting devices [30]. The most employed forms of
solid biomass fuel are pellets and briquettes [30,37].
With the target of reducing energy consumption and wear and Considering the availability of biomass resources and the effect on
deformation of key parts, relative research contents are reviewed from the local environment, different countries, areas, and institutions have
two aspects: pelleting devices and binding mechanism in this section as comprehensively set a series of standardizations from initial pelleting
shown in Fig. 2. terminologies to final pellet combustion behavior [31,37,206]. Above
In Section 2.3, there is a detailed explanation of the binding mech­ all of these, ISO 17225-2 defines several requirements and classifications
anism. It is also important to understand the fundamental mechanism of for pellet qualities destined for non-industrial (A1, A2, B) and industrial
the biomass compression process, which is required to design an energy use (I1, I2, I3), those indicators were the most used in recent papers [94,
efficient compaction equipment to mitigate the cost of production and 105] and more details can be seen as Section 4.
enhance the quality of the product [8]. Industrial densification process
mainly includes pretreatment, pelleting, and post-production [32], 3.1.2. From single pelleting press to industrial pelleting
which can be refined drying, milling, conditioning, pelleting, cooling, However, the costs of industrial pelleting experiments are higher and
and packaging processes [11,192]. Conducting industrial pelleting costs online in-time collecting of operating parameters (such as friction force
too much, so single pelleting press procedures were simplified and and temperature) is out of control for the purpose of scientific research.
adopted by the above processing [180,193]. Therefore, based on the operating principle of these traditional devices,
Research on biomass pellet binding mechanism and pelleting devices single pelleting press was introduced in lab-scale to simulate industrial
have been conducted for several years. There were some representative pelleting in pilot-scale [197,198]. Single pelleting press could be ach­
results, which are listed as following. ieved at some specific experiment factors and obtained more detailed
pelleting parameters by applying conclusions to optimize industrial
(1) Explanations of binding mechanism for pellets in the view of densification processes.
optical images [7,194]; Salas [207] and Holm [208] firstly introduced single pelleting press
(2) Illustrations of the pelleting process (compression, flow and to predict the performance of industrial pelleting. Then a model of how
friction) of industrial ring-die pelleting press [195,196]; the die friction forces are affected by the key process parameters was
(3) Pellet production model to describe pelleting pressure or force quantified through the pellet exiting pressure in single pelleting press to
along with press channel length based on single pelleting press simulate industrial pelleting [32,209]. Mišljenović [210] compared the
[24,197–199]; results obtained from single pelleting and industrial pelleting press and
(4) Structure parameter design, simulation and analysis of key parts proved single pelleting press is helpful for predicting the trend of pellet
(roller and die) for ring die pelleting press [11,199–201]; quality. Puig [211] measured friction versus die temperature curve of six
(5) Experimental measurements of torque and energy consumption types of biomass by single pelleting press, reported pellets with good
for ring die pelleting press [202–204]. quality occurs where friction decreases with die temperature and veri­
fied the results with industrial pelleting support the proposed theory.
Gong [212] reported industrial pelleting positively affected sugar yield,
3.1. Pelleting devices while single pelleting press affected sugar yield differently related to
pretreatment types and biomass species. Sun [213] established a theo­
3.1.1. Traditional industrial pelleting devices production and standards retical prediction model from single pelleting to ring-die press based on
Generally, biomass densification originated in animal feed process­ plastic mechanics, Kawakita and Heckel equations. However, some re­
ing technology, but the former needs higher stresses and lower pro­ searchers hold the opposite that there are differences between single
duction capacity under the same energy and power consumption, which pelleting press and industrial pelleting. Shang [214] argued friction
means higher strength and applicability for pelleting devices [11]. Ac­ force is the key factor when scaling up from single pelleting press to
cording to published literatures and reports [21,24,30,32,97,199,205], industrial pelleting. And the optimal parameters from single pelleting
ring die, flat die, and extruder are commercial, traditional, and con­ press may not match the industrial pelleting. Mišljenović [210] reported
ventional pelleting devices. And final productions of pelleting are there are differences in pellet quality from the two methods, which are
available in various shapes including logs, cubes, briquettes, and pellets mainly caused by pelleting procedures and fiber orientations.

Fig. 2. Organization framework to explain the pelleting process.

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H. He et al. Biomass and Bioenergy 186 (2024) 107271

Berghel [193] suggested all studies based on single pelleting press 3.2. Binding mechanism
should publish their basic information, such as parameters of the single
pelleting device (die diameter, piston diameter, piston velocity, Densification process is categorized into three stages [8,16,54,205]:
maximal pressure or force, holding time, and die temperature), prop­ particle rearrangement and volume filling under low pressure,
erties of feedstocks (particle distribution, mass, inlet moisture content, compression energy is mainly dissipated due to inter-particle and
and chemical component), which could be used to define standard set­ particle-to-wall friction in the first stage, which was called the inertial
tings for single pelleting press experiments. deformation stage; visco-elastic-plastic deformation stage of particles for
the second stage, the plasticization of condensed chemical components
3.1.3. Ultrasonic-vibration assisted (UV-A) pelleting (lignin, protein, and carbohydrate) and the non-modified chemical
It is reported that plastic transformation and flowability of components (cellulose) deformation occurs mechanical interlocking
compression materials are improved significantly with the application of under exponentially increasing pressure; and hardening into solid bridge
ultrasonic vibration [215,216]. UV-A pelleting can be achieved under and elastic spring back in last stage. Kang [38] and Sarker [39] illus­
the condition of room temperature, lower pressure, and without addi­ trated the densification process of biomass particles with figures and
tives, compared with traditional and conventional pelleting [217]. Due explained the binding mechanism from particles filling, packing, and
to the high-frequency vibrational properties and thermal effects, UV-A interlocking. Anukam [224,225] presented an analysis of a structural
pelleting has the function of mechanical compressing force and ultra­ chemistry perspective of the mechanism of bonding and discussed the
sonic vibration heating, which is helpful for binding in pelleting. effect of additives in densified biomass pellets. Above all, research on
The whole layout and assembly units of UV-A pelleting press were binding mechanisms for pellets is mainly discussed from theories and
reported by Tang [218]. Based on UV-A pelleting, the effects of input experiments. The former tried to explain the whole pelleting processing
variables (ultrasonic power, pellet pressure, pellet weight, and moisture by visco-elastic-plastic mechanics, the latter were presented by
content) for inside temperature distribution of pellet during the pellet­ advanced analytical instruments and optical images.
ing process were investigated, and the highest temperature appeared at
the central of the pellet, while the lowest temperature appeared at the 3.2.1. Equations and models of densification
edge on the bottom surface. Li [219] studied the effects of different input
variables of pelleting factors on charring ratio and pelleting tempera­ (1) Constitutive models
ture. Zhang [217,220] studied the effects of pelleting factors on chem­
ical components and sugar yield for corn stover and sorghum stalk and Researchers tried to capture the compression behavior of biomass
verified UV-A pelleting not only produces higher density but also breaks feedstocks by constitute models, which are systems of fundamental
the lignin shell to increase cellulose accessibility and then increases rheological elements in parallel and serial configurations to describe
sugar and biofuel yield. Meng [221] investigated the potential of UV-A stress-strain relationship during densification process [144]. Rheolog­
pelleting as pretreatment method to produce biochar with multi-layer ical elements are functions of stress, strain, and time to predict the
and porous structure. Yang [56] explored cellulosic bioethanol hydro­ mechanical behavior under different loading conditions. Common
lysis residue as an additive for solid fuel production by UV-A pelleting rheological elements include Spring and Coulomb friction (used for
and explained ultrasonic wave propagates through a volume of biomass, modeling ideal elastic and plastic behavior respectively, which is related
the majority of the energy of ultrasonic wave is absorbed by biomass, with stress) and dashpot (used to represent for viscous mechanisms,
resulting in a rapid temperature increase due to viscoelastic heating, which is related with time) [144,226]. Based on those basic elements,
which makes lignin softening and natural binder solid into bridge. several constitute models (Maxwell, Kelvin-Voigt, Standard Linear Solid
Summing up, UV-A pelleting has several advantages of sugar yield SLS, SLS-Maxwell, SLS- Kelvin-Voigt, Burgers, Peleg, Faborode, and
for pelleting, it is not promoted from single pelleting press in lab-scale to Kaliyan) were developed to explore the compression properties of
industrial-scale, and any detailed research and comparisons with different biomass feedstocks. Specifically Kaliyan [144] introduced
traditional pelleting methods were not reported and verified. Besides, inertia element to model the state of the initial compression, which
the density of the whole pellet unit density is not uniform, density of the corresponding to the first stage of particle rearrangement and volume
top of pellet is higher than the bottom, which also reflects the temper­ filling. Then, a visco-elastic-plastic constitutive model with five rheo­
ature distribution. logical elements of compression was developed without considering the
inertial deformation stage and effects of natural binders. Rheological
3.1.4. Key parts design for pelleting devices parameters connected with physical properties of pellets are also built,
Nielsen [11] has presented an overview of parameters of die and increasing the absolute values of elastic modulus and viscous co­
configuration and operational variables which influence the perfor­ efficient is beneficial for the strength and durability. Besides the point to
mance of the pelleting press. In addition, roller and die are key assembly distinguish inertial stage and visco-elastic-plastic stage is determined by
in industrial pelleting devices, which are also the design basis of single the changing positive pressure gradient, which is also verified by
pelleting press. For the die, parameters of press channel of die are key Crawford [227] and Li [228]. Song [229] presents a constitutive model
factors when designed, which include: diameter, length, to predict pellet density in UV-A pelleting, which can be used to study
diameter-length ratio, inlet shape, angle, and depth [222]. Distributions the influences of input variables on pellet density. Nielsen [226] pro­
(numbers and locations) of press channels in the die also have effects on posed a non-linear Maxwell representation of the SLS model and fitted to
pellet quality and whole pelleting devices. Moreover, inner surface of the experimental compression data and concluded dashpot has re­
die could be divided into active, transition, and inactive areas based on lationships with compression speed.
materials and die interacting each other [11,12]. For the roller, the most
important factor needs to be considered is the wear-resistance properties (2) Compaction equations
[199,223]. The linear velocity of both die and roller are the same, but
the diameter of die is around 0.4–0.47 times of roller, which means there Existing compaction equations were reviewed and compared for
should be enough stiffness for roller [199,203]. Gap size between die various materials (soil, metal powder, ceramic, food, feed, and biomass)
and roller usually locates at 0.1–0.3 mm, too narrow for severe wear, too [230–232]. Compaction equations are bridge functions between some
wide for poor pellet quality [199]. In the future, the main stream of die properties of powder (porosity, relative density or void ratio) and
and roller structure design is to meet the requirement of production and compaction pressure, also establish the correlation between the process
achieve customized design for pelleting devices and processes. variables and density and reflect the mechanism of sliding, rearrange­
ment, fragmentation and strain-hardening of the particles of compacting

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process [231]. Compactability and compressibility are usually used as (1) For the next generation of pelleting devices, on the one hand, the
indicator to assess the ability of materials to be compressed. The former robustness of biomass densification devices should be enhanced
refers strength changing with volume, while the latter refers volume to adapt constantly emerging feedstocks for pelleting; on the
changing with pressure. Different compaction equations focus on other hand, exploring pretreatment and densification co-pelleting
different compression parameter variables and the most act pressure or process and developing with corresponding to specific pelleting
force as inputs and density of the production as outputs. Some classic devices.
and common equations are as follows: Cooper and Eaton equation is (2) Single pelleting press is simplified from industrial pelleting press
proposed based on particle rearrangement and elastic and plastic partly for flexible experiments with less costs. Relationship be­
deformation, Walker equation elucidates the relationship between the tween single pelleting press and industrial press should be con­
volume ratio and pressure, and Kawakita equation is pure empirical nected. And industrial standard should be made to give specific
under certain assumptions [119]. These empirical equations can be used parameters of single pelleting press and experimental procedures.
to develop a relationship between process variables (pressure or vol­ (3) UV-A pelleting is a specific case of single pelleting press, which
ume) and relative density. Such as Sanchez [232] predicted density suits for pelleting in chemistry and biorefinery industry at lab-
range according to the compression pressure. Besides Tabil [8] in­ scale and proves the application of ultrasonic-vibration in pel­
vestigates changes in compact density and volume with pressures by leting successfully. Whereas, it did not have the potential to
fitting experimental data to Jones, Cooper-Eaton, and Kawakita equa­ extend in practical industrial pelleting.
tions. Guo [233] studied the compaction and relaxation properties at (4) Exploring the pelleting process have been studied from different
different pressures, moisture contents, and particle sizes. With the perspectives. For feedstock, which includes particle rearrange­
method of fitting and developing the compaction and relaxation models, ment and volume filling at lower pressure, mechanical inter­
Jones, Heckel, Panelli, and Filho equations could not successfully locking under exponentially increasing, and hardening into solid
explain the compression behavior because of lower R-square (R2); while bridge once unloading; From the point of the moving behavior of
Walker and Cooper-Eaton equations provided good correlations (R2 > feedstock in the die, which is consisted of compression, flow and
0.90) for biomass samples. And the stress relaxation curves were friction subprocesses; Based on visco-elastic-plastic mechanics,
affected by the initial preset compression load. Wang [234] proved force changes with displacement as linear and exponential; for
Peiyun Huang equation presented the best fit for the compacting force stress-strain relationship, which contains inertial deformation,
during the whole pelleting process, followed by Kawakita and Heckel visco-elastic-plastic deformation and elastic spring-back stage.
equation. For the latter two, the fitting results were better when dealing (5) Theoretical analysis of binding mechanism of pellets has been
with the data under high compacting forces. A predictive compression explained deeply and verified by characterization technique.
model for feed based on the Kawakita and Cooper-Eaton equations was Both can be used to instruct and optimize the design of roll die
developed by Sun [235]. structure. More advanced analytical techniques can be used to
characterize the internal structure of pellets and improve pellet
3.2.2. Characterization technique quality in further studies.
Kaliyan [194] investigated the binding mechanism of corn stalk and
switchgrass pellets from single pelleting and ring-die press by light mi­ 4. Evaluations of pelleting process factor and pellet quality
croscopy (LM), scanning electron microscopy (SEM), and ultraviolet
auto-fluorescence, respectively. The SEM images showed that As shown in Fig. 3, pelleting factor variables and their influences on
particle-particle bonding mainly through solid bridges. And the physical, mechanical, thermochemical, and combustion character­
auto-fluorescence images proved the solid bridges were mainly formed istics of pellets have been reviewed from feedstock properties, process­
by natural binders such as lignin and protein. Based on this, Pegoretti ing parameters, and device structure and parameters in published
[236] reported the crack of pellet surface by SEM and explained how papers. Based on the literature review, several research [25,238,239,
lignin distribution influences the mechanical properties with confocal 241,242] also have systematically reported pellet qualities with specific
fluorescence microscopy. With the same methods, Chen [165] species and recipes, thus some controversial hot-topic experimental
concluded higher contents of hemicellulose and lignin have more stable factors (pelleting temperature) and quality indicators (durability, pri­
hydrogen bonds and fewer cracks. Lehmann [237] observed the ority, and water sorption) are just emphasized and discussed in this
cross-section and side views of miscanthus pellet to obtain the fibrous section.
structure by LM. Then Kirsten [192] proved fiber length has effects on its
interlocking bonds and gaps. Castellano [58] noticed woody feedstocks 4.1. Factors and their effects on pellet processing and quality
have a more evident deformation while herbaceous materials preserve
their shape with SEM images. Siyal [89] compared and listed the ranking of pellets based on their
Seraj [179], Azargohar [238] and Sarker [152,239,240] introduced quality parameters and energy consumption. Yılmaz [13] studied the
micro-computed tomography (CT) to explore the internal structure comparison of fuel qualities with basic physical indicators and their
(porosity and diameters of cavity) of biomass pellet, and the compliance with EN plus standards, and marked from production effi­
three-dimensional model of pellet was reconstructed and visualized. ciency, physical quality, and fuel properties. According to Mišljenović
Image J, NRecon, and Avizo software packages were used for data [210], some indicators (bulk density and durability) of pellets produced
analysis in this research, which means the calculated values of porosity by single pelleting press and industrial pelleting were not the same,
depend on the apparent color of pellets, the default setting threshold of because single pelleting press with low production rate could not meet
the image and even the lighting intensity while collecting. Thus, relative the test requirements. Nielsen [243] investigated effects of fiber orien­
values of porosity were just reported, but specific density of pellets was tation and showed transverse fiber orientation is benefit to improve
not published in previous studies. Further relationships such as between compressive strength with lower energy consumption than longitudinal.
porosity and combustion performance also need to be discussed. Eisenbies [126] proposed rapid assessments of feedstock properties and
pellet quality used to be adjusted pelleting process, classified pellet
3.3. Summary grades and meet market requirements respectively. Nielsen [11]
concluded parameters and variables affect the pelleting process, and
The main conclusions of this section are listed as follows. parameters are controllable inputs, while variables change with
parameter settings. Mostafa [35] presented an overview of the effect of
properties, adhesives, moisture, pressure, and temperature on the

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Fig. 3. Framework systems to clarify the relationship between affecting factors and pellet quality indicators.

physical and mechanical properties of the pellets and also discussed the
Table 4
interaction effects of those factors. Gong [21] discussed how densifica­
Comprehensive evaluation indicators for biomass pellet qualities.
tion process variables affect pellet qualities. Kang [38] claimed a
comprehensive index system has been built to evaluate pellet qualities, Physical and mechanical properties Ref.

which includes physicochemical properties and additive characteristics, Pellet size (Diameter and length) [37]
pellet stability, binding mechanism, and combustion characteristics. Dimensional expansion [246]
Compacted/Relaxed density [129]
Above all, researchers have been devoted to establish relationships be­
Mass yield [247]
tween process factors and pellet qualities and there has been systematic Specific energy consumption [195]
and theoretical basis. Based on those published reviews, factors and Durability [31]
indicators during the pelleting process were reviewed in Tables 3 and 4. Tensile strength [175,180]
However, with the densification technologies developed, some factors Compressive strength [241,242]
Mayer hardness [165]
and indicators need to be surveyed once again, thus differences of the
Drop test [248]
pelleting temperature and pretreatment temperature, porosity and hy­ Water sorption [248]
drophobicity of biomass pellet were discussed in the following Hydrophobicity [152,165]
subsections. Water absorbability [153]
Water resistance/Moisture absorption [168,249]
Wettability index [87]
4.2. Pelleting temperature and moisture content of feedstocks Thermochemical property/combustion characteristics [178]

Thermogravimetric analysis [180]

Many studies have been conducted to investigate effect of the tem­ Heating value [130,250]
perature and moisture content on pellet qualities. Kaliyan [194] pro­ Ash content [251–254]
posed proper moisture and temperature to activate natural binders of Major elements content [67,255,256]
feedstock have beneficial to make durable pellets. As reported moisture
content of feedstocks in industrial pilot scale (10–25 %) usually is higher
for pelleting, which is also line with most researchers reported at pre­
than those in single pelleting press (10–15 %). Uslu [17] concluded
sent. Water could act as binder during densification, too dry or too wet
moisture content of feedstocks ranging 10–25 % is considered optimal
of feedstock will increase required pressure for pelleting. García [94]
studied effects of temperature (50–80 ◦ C) and moisture content (14–20
Table 3 %) on pellet quality, and the best pellet quality was obtained with
Factor variables influence on pelleting process and pellet quality.
moisture content of 16.6 % at 80 ◦ C. Mohamed [35] reviewed the effects
Factor variables Ref. of die temperature and moisture content of feedstocks on the dimension,
Feedstocks density, durability and energy consumption of biomass pellets in detail.
Physical properties [35,241,244] According to reports by Nielsen [11], pelleting temperature was
Particle size [58,192,237,242] determined by moisture content, inlet temperature and friction in the
Particle shape [45]
press channel of feedstocks. For industrial pelleting, moisture content
Moisture content [81]
Chemical components [33,35,245] and inlet temperature of processes were controlled by conditioning
Cellulose/hemicellulose/lignin/extractives process, and pelleting temperature was arising to 120–130 ◦ C because of
Pelleting process the friction caused by feedstocks and press channel of die, and the
temperature near the roller is higher than the far one up to 135 ◦ C [243].
Operating variables [34]
Applied pressure/force [246]
The pelleting temperature decrease from near to far the roller also re­
Die temperature [57,247] flects the dissipation of energy by expelling pellets out bring heat during
Retention time [35,113] pelleting process. And for single pelleting press, controlled heating de­
Compressive rate/speed of die [202] vices were added to increase pelleting temperature and simulate the
Device structure and parameters
industrial pelleting process. Besides, pelleting at room temperature is
Design of die [11,200,201]
Design of press channel of die [197] always reported as control group. Stelte [7] and Nurek [77] conducted
Gap between roller and die [11,199] pelleting experiments at different temperature (20, 100 ◦ C) and (22,

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H. He et al. Biomass and Bioenergy 186 (2024) 107271

73 ◦ C) respectively in single pelleting press and reported pellets pro­ pellet indicates lower mechanical strength. Siyal [89] used relaxed and
duced at higher temperature has better performance. San [90] investi­ true density of pellets to determine the porosity, and discussed effects of
gated effects of pelleting temperature (20–300 ◦ C) and pressure temperature and pressure on porosity.
(30–208 MPa) on durability and density of pellets. Another indicator of pellet quality needs to be considered is the
Based on binding mechanism and chemical component of feedstocks, surface crack of pellets, which reflects the durability of pellet, the
pelleting temperature is usually associated and compared with glass adoption between pelleting process and biomass feedstocks and the
transition temperature (Tg) of feedstocks. Stelte [7] referred range of stress relaxation of feedstocks after pelleting. According to Rezaei [109],
softening temperature of biomass feedstocks as Tg. Above the tempera­ the surface quality of biomass pellets are mainly consisted of cracks,
ture point Tg, state of chemical components will change from glassy into fissures, and roughness. Mišljenović [210] measured roughness of pellet
rubbery. Below the Tg, those will be recombined into solid bridge [194]. surface with profiler and reported contact angle of pellet and water drop
Common and typical value of Tg is in the range of 50–140 ◦ C for biomass by optical devices. Pradhan [24] attributed the cracked pellet surface to
feedstock [11]. Mišljenović [210] reported binders play a leading role high moisture content of biomass feedstocks, which is consistent with
when pelleting temperature is lower Tg. Yang [257] reported pyrolysis Anukam [224].
temperature of hemicellulose was focused at 220–315 ◦ C, cellulose was On the one hand, with the market supply demand, biomass pellets
mainly happened at 315–400 ◦ C, while lignin covered the whole tem­ under transport across oceans and storage in humid environments also
perature range 150–900 ◦ C. Therefore, there is a need to classify tem­ need to be considered. On the other hand, with the popularization and
perature point of pelleting, torrefaction and pyrolysis. Taking Section development of pretreatment technologies, biochar pellets are
2.5.2 as reference, temperature of pyrolysis is higher than pelleting increasing production. Thus, water sorption of biomass pellet indicator
temperature, while torrefaction temperature has similar range, it seems is proposed as shown in Table .4, which can also be called hydropho­
combining torrefaction and pelleting as a promising technology. bicity, water absorbability, water resistance, moisture absorption, and
Puig [211] observed the effects of pelleting temperature on friction, wettability index. Testing methods and devices differ depending on
which increased from 20 to 90 ◦ C and then decreases from 90 to 120 ◦ C experimental conditions and targets in published papers. No more
and concluded rising friction contributes to enhance pellet density and comparable information can be used, thus there is urgent to make the
also increases energy consumption. Zhang [258] simulated temperature indicator unified. Liu [177] and Jiang [117] used the ASABE S358.2 to
and friction rising with time by spatio-temporal model and verified by measure equilibrium moisture content as moisture absorption at the
pelleting experiments to clarify heat transferring mechanism in single earliest. Recently ISO 23343–1 was published for the determination of
pelleting press. water sorption of biomass pellets in a laboratory setting and explained
how durability of pellet was affected by immersing in water. Therefore,
4.3. Durability, porosity, and water sorption of pellets water sorption of biomass/biochar pellets should be conducted based on
the standard to make results for reference and comparability.
Mechanical durability is the most noteworthy indicators of pellet
quality to evaluate the resistance of pellets breaking into dust and fines 4.4. Techno-economic analysis (TEA) and life cycle assessment (LCA) of
during transportation, which is originated from the pellet durability pellets
index (PDI) [11,31]. Based on reported results, durability is affected by
chemical components of feedstocks and pelleting process and has posi­ Conducting TEA and LCA of biomass pellets enables systematic
tive relationship with pellet density. Different industrial standards (ISO analysis of the relationships between technical, economic, and envi­
17831–1, ISO 23343–1, EN 15210–1, and NY/T 1881.8) have enacted ronmental performance [17,260]. Muazu [261] proposed densification
elaborate measuring steps for durability. And there are also different is a worthwhile process for biomass energy conversion systems and
testing devices and methods such as tumble tests, drop tests [168], and could reduce net energy consumption by 200–1000 kJ MJ− 1 and GHG
Ligno tests [31]. However, all those are for pellets from industrial pel­ emissions by 9–50 CO2-eq (g MJ− 1) varying with different feedstocks.
leting, and pellet productions of single pelleting press could not reach Silva [262] discussed the effects of pellet and briquette production on
the amounts (500 g for every single test) of durability [31,210]. the environment in various scenarios and explained the great potential
Therefore, different definitions of single pellet durability (maximum political implications of expanding emission trading systems in Latin
compression force [78,259], compressive/tensile strength [241,242], America. Martín [263] found differences in methodological choices on
and Meyer hardness [54,117,165], as shown in Table .4) were used to life cycle impacts, suggested a consistent and robust framework for the
replace industrial durability for single pelleting press in lab-scale. Be­ harmonisation of LCA results, and proved correlations between global
sides, Liu [127] randomly selected and weighed pellets from single warming and non-renewable primary energy. Hamedani [264,265]
pelleting press and then put them in vibrating sieve with certain screen evaluated the vine, olive grove, and coffee ground pellet production
size for 10 min to calculate mass loss of samples as durability. Larsson from cradle to grave by LCA, and indicated agricultural operations and
[31] and Yu [19] conducted single pellet durability tests compared with the pelleting process mostly impose all environmental burdens. Guo
ISO standard durability and relationships of both could be seen as linear [153] also reported corn planting and pelleting process are the main
at some specific experimental conditions. So, there are still differences contributors to energy consumption in the whole life cycle of pellet fuel
between single pellet durability and industrial durability, more detailed production, and energy return ratio also increased with the ratio of coal
industrial standards for the pellet indicator “durability” should be dis­ cutting waste. Cen [266] investigated the energy flow of torrefied
cussed and explored to be normalized, and obtained results could be cornstalk pellets in the combustion heating system by LCA, and showed
transferable and comparable in the future for single pelleting press in acidification and photochemical smog are the main environmental
lab-scale and industrial pelleting in pilot-scale. impacts.
Porosity of biomass pellets can be used to instruct storage and García [108] analyzed the costs of grinding, transporting, and con­
transport, especially for the combustion characteristics. Benefiting from structing increased while the overall pellet production cost decreased
advanced analytical instrumental techniques (seen as Section 3.2.2), with the addition of cost-less RDF. Considering the costs of feedstocks,
Muazu [146] and Sarker [240] respectively introduced CT to the pel­ additives, pretreatments, pelleting, transport, and storage, torrefied
leting industry and used internal porosity as an indicator to evaluate the pellets are competitive for big installations and long-distance transport
pellet quality. The porosity was calculated as the ratio between volume [95]. In terms of economic indicators (payback period, return on in­
of void space and the volume of the sample pellet cylinder [146]. Sarker vestment, and the internal rate of return), Agar [173] proposed torrefied
[240] also held that porosity measurement has positive with the density pellets have no competitive advantages with the conventional. Ståhl
and mechanical strength measurements of pellets, higher porosity of [267] reported using cornstarch and molasses as additives decreased

12
H. He et al. Biomass and Bioenergy 186 (2024) 107271

energy consumption and the CO2 eq. mitigation, as well as increased the organization. However, Chen [165] defined in-situ and ex-situ torre­
durability of pellets and customer satisfaction. Wang [150] proposed faction densification as: in-situ is binder free process and without cool­
starch as binder is the first choice when considering the economic ing; ex-situ refers biomass densification after traditional reprocessing
analysis. with binders.
Von [268] found wild plant species are economically viable for pellet Research dominated by big data and algorithms to assess pellet
combustion because of low cultivation costs, availability of subsidies, quality is increasing with the development of pellet production line
and low pellet production costs due to low moisture content. Pajampa industrialization and quality management systems for enterprises. Ma­
[269] conducted an economic analysis of filter cake pellets for steam chine learning techniques were used to classify pellet quality by spectra
power plants to reduce the cost of feedstock and logistics with significant obtained using near-infrared spectroscopy [273]. Pierdicca [274]
profits. Stachowicz [270] proposed the cost and energy intensity of short developed a deep neural network architecture to determine the
rotation coppice and their mixture pellet production accounted for geometric-dimensional parameters of wood pellets. You [275] used
50.3–57.8 % and 74.6–82.6 %, respectively. Gul [28] reported using manufacturing parameters, feed formulation, and environmental data to
biocarbon pellets in the steel industry can bring some environmental build machine learning regression models for pellet quality prediction.
advantages, but economic and energetic feasibility needs to be opti­ Moreira [276] assessed the production of high-performance fuel-flexible
mized. Ningsih [151] calculated the economic feasibility of pine flower woody pellets for heating and power by multivariate statistical process
briquette production, the profit on sales, rate on investment, pay out control.
time, and break event point were 26.43 %, 34.00 %, 2.47 years, and
49.22 %, respectively. 6. Conclusion

4.5. Summary This paper systematically reviews biomass densification technologies

as well as involves relative research from feedstocks to pellets.
Some conclusions and prospects of this section are presented as Remained issues in every single industrial processing for pelleting are
follows. concluded, with corresponding suggestions and comments are given.
Overall biomass densification technology is a multidisciplinary subject,
(1) Research has been systematically conducted about affecting fac­ which involves mechanics, materials, biological chemistry, thermody­
tors (especially for pelleting temperature, moisture content, and namics, and environmental science. And biomass pelleting needs treat­
particle size of feedstock) and pellet qualities (density, durability, ments in accordance with local conditions for specific regions, which is
and energy consumption). Even multi-parameter models of fac­ also why it got so rapid development in the past decade. With advan­
tors and indicators for various feedstocks have been established tages of bioenergy itself and developments of some rising pretreatment
under different experimental conditions. Results showed mois­ technologies, those co-pelleting or co-processing with densification will
ture content at 10–15 % and pelleting temperature ranging from be applied more scenarios in the future. Biomass should be brought and
70 to 100 ◦ C have the best pellet qualities and combinations of utilized for local energy supply first and ensured have no effects of time
different particle sizes also perform better. However, there are and season. Under this circumstance, with the target of comprehensively
still gaps in making results from single pelleting press in lab-scale increased utilization of biomass and improvements for pellet quality,
and industrial pelleting in pilot-scale comparable and research should be conducted in more elaborate domains.
predictable.
(2) Temperature points of densification, torrefaction, and pyrolysis CRediT authorship contribution statement
need more attention. Based on the above, more co-processing of
pretreatment and densification can also be developed to optimize Haomeng He: Writing – review & editing, Writing – original draft,
pelleting process and enhance the utilization of biomass Methodology, Investigation, Conceptualization. Yu Wang: Writing –
feedstocks. review & editing, Writing – original draft, Methodology, Conceptuali­
(3) Comprehensive standards from feedstocks to pellets have been zation. Yu Sun: Writing – review & editing, Writing – original draft,
drawn up to guarantee the regulation of the biomass pellet in­ Methodology, Conceptualization. Wanfeng Sun: Methodology, Inves­
dustry and environmental safety. However, some indicators need tigation, Conceptualization. Kai Wu: Writing – review & editing,
to be updated with the tendency of biomass pellet industry, such Writing – original draft, Methodology, Conceptualization.
as the described definition and testing methods of durability need
to be adjusted in line with the requirement of single pelleting Acknowledgements
press; priority and moisture adsorption should be raised for
biomass pellet productions. This work was supported by the Natural Science Foundation of
(4) Energy consumption, economic benefits, and environmental im­ Jiangsu [BK20190473].
pacts of biomass pellets are attributed to the processes of trans­
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