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Densification of waste biomass for manufacturing solid biofuel pellets: a

review

Article  in  Environmental Chemistry Letters · September 2022

DOI: 10.1007/s10311-022-01510-0

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Environmental Chemistry Letters
https://doi.org/10.1007/s10311-022-01510-0

REVIEW

Densification of waste biomass for manufacturing solid biofuel pellets:

a review
Tumpa R. Sarker1 · Sonil Nanda1 · Venkatesh Meda1 · Ajay K. Dalai1 

Received: 22 August 2022 / Accepted: 27 August 2022

© The Author(s), under exclusive licence to Springer Nature Switzerland AG 2022

Abstract
The demand for bioenergy is increasing due to the diminishing popularity of fossil fuels and rising greenhouse gas emis-
sions. However, according to recent reports, renewable energy sources account for only 14% of the total primary energy
supply, of which bioenergy accounts for 67%. Densification of biomass offers a sustainable pathway to generate solid fuels,
which can replace coal while liberating bioenergy, reducing carbon emissions and valorizing organic wastes. Because of the
rising demand for fuel pellets, there has been an increased interest in utilizing a wider range of biomass resources. Density,
mechanical stability, hydrophobicity and energy content are the major properties controlling the quality of fuel pellets. These
properties are influenced by biomass type, pretreatments, formulations such as binders, additives and lubricants, densifica-
tion methods and conditions including temperature, pressure and relaxation time. Here we review biomass densification,
mechanisms, factors affecting the pelletization process and pellet quality, and characterization techniques to access the fuel
quality of pellets. Furthermore, we present additives, binders and lubricants used for the pelletization of a wide variety of
biomass. This review also identifies the major applications for fuel pellets.

Keywords  Additives · Biofuel · Biomass · Characterization · Densification · Fuel pellet · Pelletization

Abbreviations s Seconds
% Percent wt% Weight percent
°C Degree Celsius
g/mol Grams per mole
GJ/m3 Gigajoules per cubic meter Introduction
h Hour
kg/h Kilogram per hour The rising demand for world energy increases the exten-
kN Kilonewton sive usage of fossil fuels which emit massive amounts of
m Meter ­CO2 leading to environmental pollution and climate change
M Million (Fawzy et al. 2020; Chen et al. 2022a, b). It is esti-
mg/m3 Milligram per cubic meter mated that energy demand will rise by 19% across the globe
min Minutes by 2040 (IEA 2020), which follows an annual increase in
MJ/kg Megajoules per kilogram ­CO2 emissions by 1.9% over the last few decades (Chen
mm/min Millimeter per minute et al. 2016a). To reduce the dependency on fossil fuels and
mm Millimeter mitigate the negative impact of their burning, research and
MPa Megapascal development of alternative fuels are highly essential. This
N Newton could allow for the utilization of easily available renewable
rpm Revolutions per minute resources with minimal or no negative effects on human or
animal health and the environment. Moreover, it has been
agreed in the Paris Agreement followed by the 2021 United
* Ajay K. Dalai
ajay.dalai@usask.ca Nations Climate Change Conference (COP26) to achieve
net-zero emission by mid of century and limit the world
1
Department of Chemical and Biological Engineering, temperature rise to 1.5 °C (COP26 2022).
University of Saskatchewan, Saskatoon, Saskatchewan,
Canada

13
Vol.:(0123456789)
 Environmental Chemistry Letters

Biomass is the most promising substitute for fossil fuels the densification of biomass followed by the application of
to produce usable forms of solid, liquid and gaseous energy fuel pellets.
carriers in contrast to other renewable sources such as solar,
tidal, wind and geothermal resources. Furthermore, using
agricultural residues and organic wastes as substrates to gen- Potential of biomass for densification
erate biofuels can cut down the greenhouse gas emissions
from landfills and open burning, thus providing a revenue Figure 1 depicts different second- and third-generation bio-
stream for biomass suppliers. According to Global Bioen- mass resources as potential precursors for biofuel produc-
ergy Statistics 2020 reports, renewable energy sources con- tion. It is worth mentioning that starch-based materials such
tributed almost 14% of total primary energy supplies in 2018 as grains, corn, potato and cassava are referred to as first-
of which bioenergy accounted for 67% (World Bioenergy generation biomass. The first-generation feedstocks encoun-
Association 2020). Biofuels can be defined as the energy ter controversies of food versus fuel, competition for arable
carrier derived from different biomass sources via mechan- lands, irrigation water and nutrient use. The second- and
ical, thermal and biological conversion routes (Demirbas third-generation feedstocks do not contend with the food
2009). Biofuels generated from waste biomass provide direct supply, cultivable lands and available water since they com-
and long-term environmental advantages as a critical com- prise mostly the inedible residues from agriculture, forestry,
ponent of sustainability (Srivastava et al. 2020; Tang et al. cattle farming, marine ecosystems, municipal solid waste
2020; Osman et al. 2021). and waste management facilities (Nandhini et al. 2022).
Some intrinsic properties of biomass such as high vol- Agricultural and woody biomasses are mainly referred to as
ume, low density, hydrophilicity, high volatile content, lignocellulosic biomass made up of cellulose, hemicellulose,
high moisture content, low energy content and heterogene- lignin and extractives (Spiridon 2020; Kaloudas et al. 2021;
ity limit its direct usage for biofuel production. Biomass Pattnaik et al. 2021). The second- and third-generation feed-
with low density and voluminous nature requires high stor- stocks can be converted into a variety of biofuels, biochemi-
age space and high transportation costs. Densification of cals and bioproducts using thermochemical, hydrothermal,
biomass reduces the cost of transportation of raw biomass chemimechanical and biological conversion technologies
by increasing bulk densities, allowing for long-term stor- (Aravind et al. 2020; Nanda and Berruti 2021b, c).
age (Bajwa et al. 2018). In comparison with other biofuels, As can be seen in Fig. 2, the production and applica-
pellets from biomass have several advantages in the large tion of biofuels are regarded as carbon-neutral, whereas the
market already including a fairly simple processing tech- integration of biochar or carbonized biomass can make the
nique and a large supply of feedstock (Kang et al. 2019). In biorefinery process carbon-negative (Balajii and Niju 2019;
addition, the demand for wood pellets for heating and power
production is steadily rising around the world in both rural
and urban communities. The global wood pellet demand for
heating is expected to reach 26 million metric tons in 2027
(Canadian Biomass Magazine 2021). The world pellet pro-
duction in 2020 was led by European Union followed by
North America, China and South America with 13, 11, 10
and 4.4 million metric tons, respectively (Statistica 2020).
Much research has been carried out on the densification
of different biomasses for fuel pellet production, but there
is little literature is available on standardization of the den-
sification process, optimization of its parameters, types of
equipment used, the mechanisms of pellet formation and
characterization techniques for determining pellet quality.
In addition, the literature on the value-added applications
of densified biomass, factors affecting biomass pelletiza-
tion and pellet quality, detailed binding mechanism during
densification and economic viability requires a thorough
update with the recent research work conducted in these
areas. This review aims to fill these knowledge gaps. A sys-
Fig. 1  Second- and third-generation feedstocks with potential for den-
tematic discussion of the evaluation techniques for pellet sification. Examples of next-generation bioenergy feedstocks include
quality is extensively made in this article. This review also agricultural biomass, woody residues, livestock manure, marine bio-
explores various binders, additives and lubricants used for mass, food waste and municipal solid waste

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Environmental Chemistry Letters
Gunarathne et al. 2019; Patra et al. 2021; Akhil et al. 2021).
The valorization of waste biomass to produce bioenergy in
addressing clean energy and greenhouse gas emissions can
support several of the United Nations Sustainable Devel-
opment Goals, especially Goal 7 (Affordable and Clean
Energy), Goal 12 (Responsible Consumption and Produc-
tion) and Goal 13 (Climate Action).
Because of the massive market potential, biomass pelleti-
zation has gained a lot of interest in academia as evidenced
by the periodic publications in the literature over the last
decade. Pellets are ideal for co-firing with coal and direct
combustion in coal pulverization systems as they are easy
to grind (Whittaker and Shield 2017) making them a cost-
effective method of reducing C ­ O2 emissions from coal-fired
power plants (Stelte et al. 2012b). However, because of their
composition, pellets break down into smaller particles and
fines when they are either made poorly with compromised
Fig. 2  Carbon–neutral and carbon-negative approaches for biomass
production and biofuel utilization. Note that ­CO2 can be fixed by
plants during photosynthesis and form cellulose, hemicellulose and
lignin, which can be extracted and converted to biofuels. The com-
binder and filler or stored incorrectly to absorb moisture.
The biomass or char fines generated from biomass pellets
can have serious health and safety consequences. The dust
accumulation from these fines on hot surfaces can lead to
explosions during bulk storage and transportation (Whittaker
and Shield 2017). The quality of the pellet depends on all the
processes carried out throughout its production processes.
A typical densification process includes the collection of
biomasses, drying, reduction of the size of particles, pre-
treatments, conditions for pelletization, densification and
bulk storage (Fig. 3).
bustion of biofuels produced C­ O2, which is consumed by the plants
again during photosynthesis. Biochar is a stable carbon obtained dur-
ing biomass conversion that can sequester carbon for longer periods
13
 Environmental Chemistry Letters

Binding mechanism during pelletization

It is important to understand the phenomenon of particle

bonding during pelletization as pellet properties especially
durability, density and mechanical strength directly depend
on the particle bond of biomass. Bonding between particles
during compression and its influence on fuel pellet quality
have not been explored extensively and well documented.
However, researchers explained the basic mechanism of par-
ticle bonding focusing physical property of biomass. Natu-
ral adhesion forces of biomass particles make close contact
during densification, whereas mechanical force drives them
to interlock.
Fig. 4  Particle compaction as a function of time and pressure during
Densification of biomass can be divided into three indi- biomass densification. Biomass particles can undergo different con-
vidual stages including the rearrangement of particles, plas- figurations during densification as impacted by pressure and time
tic and elastic deformation as well as the mechanical inter-
locking of particles as presented in Fig. 4 (Tabil et al. 2011b;
Kang et al. 2019). At the very beginning of the densification surface area resulting from the breakdown of larger parti-
process, a low compaction force is applied to the biomass cles to smaller ones. Moreover, electrostatic force and Van
particle causing rearrangement of the original slackly packed der Waals forces are activated to link the particles together
particle to produce a dense mass. In this dense mass, most (Fig. 5). Finally, the density of the produced material reaches
of the biomass particles retain their original properties and the true density of the elements after a significant reduction
energy owing to the friction between particle-to-particle in volume.
and particle-to-wall. The gap between the particles greatly Because of the diminished number of cavities, the
decreases and the space between adjacent large particles is deformed and fractured particles can no longer alter their
occupied by small particles causing the particles to become position by introducing material interlocking between parti-
immobile. Secondly, with increasing pressure, the particles cles. Moreover, the formation of the solid bridge may also be
are pushed against each other and flex plastically and elas- responsible for particle bonding during densification. These
tically, significantly increasing inter-particle contact and solid bridges may form during densification via chemical
reactions, solidification, sintering, hardening of binder or

Fig. 3  Typical steps in a pelletization process. Different steps involved in the pelletization process include biomass drying, size reduction, pre-
treatment, pellet formulation, pelletization and pellet cooling, collection and storage

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Environmental Chemistry Letters
Fig. 5  Stages in biomass densification. Note the distinction between the pre- and primary densification stages where the biomass particles
undergo free movement, volume reduction, deformation, splitting and particle interlocking
Fig. 6  Types of particle bonding during biomass densification (Origi-
nal hand drawn artwork by Dr. Sonil Nanda). The illustrations indi-
cate different configurations of biomass particles and binders through
material interlocking and solid bridge formation mechanisms
natural binding agent, hardening of molten components such
as lignin and proteinaceous compounds, starch and crys-
tallization of dissolved materials (Ibitoye et al. 2021). The
melting point of particles lower down at high temperatures
and pressure which accelerates them to migrate closer to
each other, thus increasing the contact area and shifting the
melting point to a new equilibrium level (Crawford et al.
2016; Tumuluru et al. 2016). Additionally, the glass transi-
tion materials included in biomass particles solidify as a
result of compression and heating resulting in the formation
of solid bridges.
Figure 6 shows the particle bonding during the densifica-
tion of biomass. It has also been reported that only material
interlocking bonds without involving atomic forces play a
minor or non-existent part in the overall strength of pellets
(Anukam et al. 2021). Material interlocking is not enough
in providing adequate strength for pellets due to a lack of
interaction between intermolecular and intramolecular,
which are common atomic forces induced by chemical reac-
tions. Therefore, other than the phenomenon of adhesion and
cohesion, attraction forces between solid biomass particles,
capillary pressure, solid bridge and material interlocking,
the knowledge of structural chemistry including sources of
intermolecular bonds and how they are influenced by pellet-
ing conditions is also vital to understand the binding mecha-
nism as the type of attraction forces significantly enhances
by polar functional groups present in biomass (Kaliyan and
Morey 2010; Liu et al. 2014). The existence of polar com-
pounds containing hydroxyl, carbonyl and carboxyl func-
tional groups in biomass structure could strengthen the inter-
molecular arrangement via hydrogen bonding or Van der
Waals forces through robust electrostatic attraction (Stelte
et al. 2012b; Crawford et al. 2016). The oxygen-containing
functional groups have the potential to form strong bridges
on the contact surface areas of adjacent particles (Liu et al.
2014).
Factors affecting pelletization and pellet
quality
Moisture content
Various factors influence both pellet quality and the pel-
letization process as shown in Fig. 7. The moisture content
of biomass plays a vital role in fuel pellet quality as it
directly affects the pellets’ mechanical strength and dura-
bility (Kaliyan and Morey 2010; Liu et al. 2014; Canadian
Biomass Magazine 2021). Pellets having high moisture
content attract microbial activity and easily degrade and
also increase the storage and transportation cost (Nielsen
et al. 2009; Azargohar et al. 2018). Moisture can act as
a natural binder during pelletization by providing lubri-
cating effects in reducing friction (Samuelsson et  al.
2009). In addition, during pelletization, moisture content
enhances protein unfolding, gelatinization of starch and
solubilization of fiber (Samuelsson et al. 2012). On the
other hand, higher moisture content allows expansion after
pellet production resulting decrease in relaxed density
and durability (Adapa et al. 2011). In contrast, the glass
13

Fig. 7  Factors affecting pellet quality and extrusion friction. The fac-
tors affecting biomass densification can be broadly categorized under
biomass properties such as particle size and composition as well as
extrusion parameters such as temperature, pressure, binders and lubri-
cants
transition temperature of lignin decreased at high mois-
ture content which enhances the particle bonding (Stelte
et al. 2011c). Therefore, it is necessary to find out the suit-
able moisture content of feed materials during densifica-
tion because beyond this moisture content, pellet quality
begins to deteriorate (Samuelsson et al. 2012; Kaliyan and
Morey 2009). It is suggested that moisture content above
20% produces weaker wood pellets by replacing hydro-
gen bridges between wood polymers with water molecule
bonds (Nielsen et al. 2009; Stelte et al. 2011c).
Samuelsson et al. (2012) studied the optimum moisture
content for the sawdust pellets as 11–13 wt%. Mani et al.
(2006) stated that moisture content increases the Van der
Waals forces between bonding and the surface contact
area of biomass particles while investigating the effect of
moisture on pellet quality produced from the agricultural
residue (barley straw, wheat straw, switch grass and corn
stover) and reported that density and durability increased
with the decline in moisture content. Carone et al. (2011)
explored the consequence of moisture content for olive
pruning trees by varying the moisture content from 5–20
wt% and observed that good quality pellets were obtained
at lower moisture content. A decrease in moisture content
increased pellet density and restricted dimensional expan-
sion for wheat straw and poplar wood, while the moisture
content varied from 9 wt% and 15 wt%. Puig-Arnavat et al.
(Puig-Arnavat et al. 2016) found that 10 wt% moisture is
optimum for six different biomass such as alfalfa, fescue,
Miscanthus, sorghum, willow and triticale.
Several studies have also been carried out and found a
link between biomass moisture content and the mechani-
cal stability of pellets. A positive correlation was noticed
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Environmental Chemistry Letters
between pellet durability and moisture content of biomass
(Lehtikangas 2001). Durability increased from 92 to 96%
when the moisture content increased from 7 to 12.5 wt%
for Scots pine (Filbakk et al. 2011). They also reported the
optimum moisture content as 10 wt%. The best durability
was obtained at 13 wt% of moisture for tulip wood pellet,
while an enhancing trend was observed for larch pellet when
moisture content varied from 7 to 9 wt% (Ahn et al. 2014).
The most suitable moisture content for durable pellets
from woody biomass and crop leftover especially straw
was found to be 7 wt% and 11 wt%, respectively. Moreover,
Moon et al. (2014) reported that better pellet quality was
obtained at a moisture content of 20–25 wt%. Another study
stated that the optimum moisture content of switchgrass,
Miscanthus and wheat straw was 25 wt% (Jackson et al.
2016). Alike single pellet units, several studies were also
carried out using a large pellet mill on assessing the effects
of moisture content on the quality of fuel pellet produce at
the pilot scale. Theerarattananoon et al. (2011) observed a
downward trend of pellet durability for wheat straw and corn
stover when the moisture content was beyond 14%, while
the highest durability was found in between 14 and 16 wt%
of moisture content for sorghum stalk. In another study, the
highest durability of barley straw was attained at a moisture
content between 19 and 23 wt%. They also reported that,
at moisture content below 8 wt%, a barley straw pellet was
produced in a ring pellet mill (Adapa et al. 2013).
The moisture content of biomass affects the pellet qual-
ity and pelletization process forming a solid bridge between
biomass particles by lowering down the glass transition
point of lignin and by increasing the Van der Waals forces.
On the contrary, a negative effect was also found for adding
more water. According to Nielsen et al. (2009), pellets were
weaker as they progressed from 5 to 14 wt% moisture con-
tent due to loss of hydrogen bonding. Another study found
8 wt% moisture content as optimum for quality pellets and
noticed an inverse relationship between the moisture content
of Scots pine with the durability of the pellets (Arshadi et al.
2008).
Biomass particle size
Biomass particle size and shape also influence pellet prop-
erty. The mechanical durability and density of pellets are
affected by the particle size of biomass as smaller parti-
cle size provides greater surface area during pelletization.
Small to medium size of particle provides a larger surface
area for moisture addition at the time of steam condition-
ing, which enhances the binding mechanism by improv-
ing starch gelatinization. Pelleting efficiency and cost are
improved by a particular percentage of fines to medium
particle sizes. However, too small particles might cause
pellet mills to jam and reduce manufacturing capacity.
Environmental Chemistry Letters
Yılmaz et al. (2021) studied the influences of particle
size on pellet properties obtained from greenhouse melon
stalk biomass, while particle size varied from 4 to 6 mm and
reported that the highest pellet quality was obtained at a par-
ticle size of 4 mm. They also noticed that particle size has no
significant impact on pellet durability. Rezaei et al. (2020)
explored the impact of particle size of refused derived fuel
on pelletization properties and observed that the smaller
the particle size, the higher the energy consumption. The
smaller size of the particle increases the friction between
die, thus requiring higher energy. On the other hand, a higher
particle size of biomass restricts free-flowing into the pellet
mill and may also clog inside of the channel.
Labbé et al. (2020) reported that the highest durability
can be obtained for biomass of large particle size. They also
explored the emission during combustion and observed that
particle size in the range of 3.2–6.3 mm provided the low-
est CO emission. They did not find any correlation of pellet
density with the particle size of biomass. Harun and Afzal
(2016) studied the effects of particle size of biomass on pel-
let mechanical properties while conducting studies on two
different woody biomasses such as pine and spruce and three
different agricultural residues including timothy hay, switch-
grass and reed canary grass at three particle sizes, especially
150–300, 300–425 and 425–600 µm. The study concluded
that biomass with a lower particle size produced more dense
pellets due to better particle interlocking.
Carone et al. (2011) studied how particle size affected the
durability and density of olive tree pruning residue pellets
using a single pelletizer unit while varying particle size at
hammer mill screen sizes of 1, 2 and 4 mm. A decline in
particle size caused an increase in pellet density in all situa-
tions. Ishii and Furuichi (2014) did not find any noteworthy
influence of particle size of biomass on durability and yield
ratio of rice straw pellet, while the particle size was varied
from 5 to 20 mm. However, they concluded the optimum
particle size to obtain a quality pellet was 10–20 mm.
Kirsten et al. (2016) reported a hammer mill screen size
of 4 mm to provide a high-quality pellet from hay using a
ring die press, while the particle size varied in the range of
2–6 mm. Shaw et al. (2009) stated that pellet density and
tensile strength increased when particle size was reduced
from hammer mill screen size of 3.2–0.8 mm, while diamet-
ric expansion decreased. Mani et al. (2004) noticed a similar
trend of the increment of pellet density with a decrease in
the particle size of biomass.
Serrano et al. (2011) noticed no apparent effects of par-
ticle size on pellet durability when pelletizing barley straw
using a ring die pellet mill of 100 kg/h capacity at ham-
mer mill screen sizes of 4 mm and 7 mm. Theerarattana-
noon et al. (2011) also used a ring die pellet mill to produce
pellets from wheat straw, corn stover and sorghum stalk.
They observed an insignificant influence of particle size on
the density and durability of fuel pellets. Bergström et al.
(2008) investigated the impacts of the particle size distribu-
tion of Scots pine sawdust on pelletization carried out via a
ring die pellet mill with a capacity of 300 kg/h. They con-
cluded that energy consumption and compression strength
slightly changed by particle size distribution with no notice-
able impact on pellet properties such as moisture content,
bulk and particle density, abrasion resistance and moisture
adsorption. They also recommended that crushing sawdust
particles to less than 8 mm was perhaps superfluous. There-
fore, a modest relationship between particle size and density
of pellet can be suggested. It may be inferred that reducing
the particle size of biomass below a certain threshold does
not influence the overall pellet quality.
Biomass composition
The composition of lignocellulosic biomass has significant
contributions to the pelletization process. Biomass generally
contains low molecular weight compounds including organic
and inorganic components and macromolecular compounds
such as cellulose, hemicellulose and lignin (Tumuluru et al.
2011). In terms of chemical compositions, lignocellulosic
biomass mainly contains cellulose, hemicellulose, lignin,
protein, lipid, starch, ash, water and other extractives (García
et al. 2018; Cui et al. 2021). It is important to understand
the compositional changes that occur during biomass pro-
cessing, which helps to understand the compaction behavior.
Cellulose, hemicellulose and lignin are the basic com-
pounds of lignocellulosic biomass, which make up the plant
cell wall and provide strength and rigidity to the plants.
Lignin is covalently and non-covalently attached to cellu-
lose and hemicellulose generating a complex three-dimen-
sional network. Though all plant cells make up the same
components, the level of these compounds could vary by
the stages of growth, variety or species of plant, region of
cultivation and harvesting period. Woody biomass contains
more lignin, while herbaceous biomass contains more hemi-
cellulose (Cui et al. 2021). Hardwoods have comparatively
lower levels of lignin than softwood (Zhang et al. 2012).
Similarly, the ash percentage of biomass varies significantly
from plant to plant. For example, woody biomass has less
ash content compared to herbaceous or agricultural biomass.
Plant roughly contains 10 wt% of water, but it could vary
substantially depending on their growth phase and storage
period (Zhang et al. 2012). Woody biomass has trace levels
of protein (less than 1 wt%). However, legumes and micro-
algae contain substantial amounts of protein (up to 30 wt%
or higher). These chemical compounds have a substantial
impact on the quality of fuel pellets such as density, durabil-
ity, mechanical strength and hydrophobicity as well as the
pelletization process including overall energy consumption.
13

The starch content of biomass affects the binding mecha-
nism during pelletization due to gelatinization at high tem-
peratures and pressure. It also provides lubricating effects
that result in the eased flow of biomass particles through
the extruder die (Tumuluru et al. 2011). Like starch, protein
also strengthens the interparticle bonding during biomass
densification. Protein usually undergoes denaturalization at
high temperatures, which leads to forming new bonds with
other compounds such as lipids and starch to enhance the
binding capacity. Biomass containing a higher portion of
starch or protein produces durable and strong pellets (Tabil
et al. 2011a). Fat content in biomass can make the pelletiza-
tion process smoother and less energy-intensive by provid-
ing lubricating effects. However, high-fat content negatively
affects pellet quality and weakens the bonds between bio-
mass particles due to its hydrophobic nature (Tabil et al.
2011a; Azargohar et  al. 2018). Lipids, proteins, waxes,
starch and other extractives reduce friction between the
extruder die and press channel, thereby lowering the pel-
letization pressure by creating a surface layer that acts as a
lubricant (Nielsen et al. 2009; Peter et al. 2010; Stelte et al.
2011b, 2012a).
The lignin content of biomass plays a significant role dur-
ing the pelletization of biomass by creating a solid bridge
at elevated temperatures. Van Dam et al. (2004) stated that
high lignin content produces a more durable pellet as it acts
as an intrinsic resin. Lignin allows adhesion and functions
as a strengthening and binding agent. Higher lignin levels
are thought to contribute to the durability of pellets since
it works as a glue that holds biomass particles intact. Sev-
eral researchers reported that biomass particles are mainly
attached by forming a solid bridge between natural bind-
ers such as lignin, protein, starch and other extractives at
variable pelletization temperatures and pressures. Lignin
polymers change from a glassy to a rubbery phase at high
temperatures, thus reducing polymer stiffness (Stelte et al.
2011a). Pellet quality improves as a result of the lignin glass
transition following the flow and hardening. At higher tem-
peratures, lignin in the biomass softens and acts as a binding
agent. However, the correlation between the lignin content
and pellet durability is not always linear. Lehtikangas (2001)
found an unstable link between the lignin content of bio-
mass and the durability of pellets. In contrast, pellets from
biomass containing high content of lignin and extractives
showed high mechanical strength due to enhanced interpar-
ticle bonding. Another advantage of lignin is its hydropho-
bic nature, which aids to expand storage behavior, while
hemicellulose negatively affects this property of pellet due
to hydrophilicity.
13
Environmental Chemistry Letters
Pelletization conditions
Extrusion disc temperature
Temperature is the most influential factor during the densi-
fication of biomass that greatly affects the pellet density and
mechanical strength. At a suitable range of temperatures,
natural binding agents especially lignin, extractives or other
additional binder undergo deformation resulting in better
interparticle bonding. Lignin content in biomass plays a vital
role in enhancing the binding mechanism. Lignin melts at a
temperature above its glass transition temperature and con-
tributes to the binding structure of particles, which repo-
lymerizes after cooling. Therefore, the temperature of the
extruder die should be higher than lignin’s glass transition
temperature. However, the glass transition temperature of
lignin depends on biomass composition and moisture con-
tent of biomass. Biomass containing high lignin requires
a high pelletization temperature for exhibiting plasticizing
effects and solid bridge formation to obtain high-quality pel-
lets. Hence, the pelletization temperature of woody biomass
is comparatively higher than herbaceous biomass (Cui et al.
2021). Extreme temperatures destroy the binder and biomass
components to a certain extent, while low temperatures pre-
vent the softening of binders or lignin, thereby producing
low-quality pellets. As the temperature rises, friction in the
press channel decreases, thus lowering the energy and pres-
sure needed for pelletization.
The density, durability and mechanical strength of pel-
lets have a positive linear correlation with pelletization
temperature. Ma et al. (2021a) investigated the influence of
the extruder die temperature (60–160 °C) on biomass pel-
letization. They noticed that the abrasion index decreased
at higher temperatures, while a slight decline in density was
noticed at temperatures above 120 °C. Wilczyński et al.
(2021) stated that the extruder die temperature of 150 °C
provided the highest mechanical strength for briquettes pro-
duced from sawdust by varying the temperature from 25 °C
to 250 °C. Both mechanical stability and durability of empty
fruit branch pellets were found to be significantly improved
with elevated temperature. This was because more lignin
molecules permeated the biomass particles at higher tem-
peratures to form a stronger solid bridge and crosslinked
interactions between lignin and hemicellulose (Ruksatham-
charoen et  al. 2019). However, Lisowski et  al. (2019b)
observed an inverse relationship between temperature and
pellet strength and density.
Riva et al. (2019) optimized pelletization conditions such
as temperature, pressure and binder concentration using the
Box-Behnken design based on the mechanical strength and
durability of the pellets. They reported that the best qual-
ity pellets were obtained at 60 °C. Azargohar et al. (2019a)
studied the effects of pelletization temperature on canola
Environmental Chemistry Letters
hull pellet quality by varying the temperature (85–115 °C).
They concluded that 100 °C was the optimum pelletization
temperature. Another study reported that pellet durability
and mechanical strength increased with a rise in extruder
die temperature. However, the optimum temperature for oat
hull pellets was found to be 100 °C (Abedi and Dalai 2017).
Pressure
Pelleting pressure is one of the important factors to be con-
sidered. The maximal compressive force applied by the
machine on the biomass material is known as the pelletizing
pressure. Moreover, pressure is developed due to the resist-
ance between feedstock and the press channels in the die,
which appears between the extruder die and roller during
compressing of feedstocks. Pressure during compression is
mainly developed via two mechanisms such as internal fric-
tion due to the breakage of inter-particle bonds and external
friction between the extruder die surface and biomass par-
ticles. To compress the biomass particles, a specific degree
of force needs to be applied. A better-quality pellet can be
obtained at elevated pressures. However, higher pressure
consumes high energy, and energy consumption must be
kept to a minimum while achieving the techno-economic
feasibility of the pelletization process. Herbaceous biomass
requires less energy to pelletize as they are easy to compress
compared to woody biomass (Cui et al. 2021). The pelletiz-
ing pressure applied to agricultural and woody biomasses
typically ranges from 210 to 450 MPa.
Density and compression strength were significantly aug-
mented with the rise in pressure and the optimum pressure
was 150 MPa for an optimal quality pellet, while pressure
varied from 3 MPa to 150 MPa (Wilczyński et al. 2021).
Compressive strength and durability of pellet trends to
increase with the rise in pressure to a certain point and then
decline with further increase in pressure (Riva et al. 2019).
The optimum pressure was stated as 113 °C at a varying
pressure range of 60–240 MPa.
Ma et al. (2021b) investigated the effect of pelleting pres-
sure and observed that both Meyer hardness and density
increase with a rise in pressure. However, after reaching
certain pressure (100 MPa), the rise in density was neg-
ligible. Therefore, the suitable pressure for pelleting corn
cob was 100 MPa at an experimental pressure range of
10–150 MPa (Ma et al. 2021a). However, the compressive
strength of hydrothermally pretreated biomass pellet did not
change with pressure, while raw biomass showed signifi-
cant improvement in the pellet strength (Ruksathamcharoen
et al. 2019). Azargohar et al. (2019a) reported 3500 N as the
optimal compression force for pelletization of canola hull
with the addition of bio-based additives. Abedi and Dalai
(2017) investigated the effects of pelletization pressure on
oat hull pellet quality. They observed that pellet strength,
durability and density increased when compression force
increased from 3000 to 5000 N. Another study reported that
agglomeration pressure developed during compression had
the highest influence on pellet strength compared to its den-
sity (Lisowski et al. 2019a).
Relaxation, retention and holding times
Relaxation time or holding time is the time at which the
extruder die remains when it reaches the desired pressure,
thus affecting the mechanical quality of the pellets. Abedi
and Dalai (2017) observed a slight impact of relaxation time
from 15 s to 60 s on pellet properties. Bazargan et al. (2014)
found no noticeable impact of holding time on pellet strength
at pelleting pressure of 80 MPa. In contrast, relaxed density
slightly changed when relaxation time increased from 15 s to
55 s (Azargohar et al. 2019a). Li and Liu (2000) investigated
the effects of holding time for oat sawdust and noticed that
the impact of relaxation time is high when the pelleting pres-
sure was low and no significant effects were observed above
the pelletizing pressure of 138 MPa. They further noticed a
5% increase in density for 10 s of relaxation time with no
dramatic effects after 20 s.
The density of the pellet is affected by the relaxation
time. The relaxed density of densified fuel and the relaxation
behavior of pellet is influenced by a variety of parameters
including extruder die shape, compression magnitude and
mode, feedstock type and quality, and storage conditions.
Several investigations on high-pressure biomass compaction
have suggested that as the material is removed from the die,
the density gradually reduces to a final relaxed density. The
rate of expansion for most biomasses is maximum imme-
diately after pressure is removed and diminishes with time
until the biomass reaches a steady volume.
Other significant parameters
There are some parameters of the pelletizer equipment such
as dimension and speed of the extruder die and pressure
difference between the die and roller that can affect the den-
sification process and quality of fuel pellets. The amount
of biomass material densified during pelletization is deter-
mined by the mass flow of biomass and extruder die speed.
The compression rate of feedstock is also determined by the
extruder die speed. However, the effects of these parameters
have been investigated by several researchers.
It has been reported that the specific energy consump-
tion increased with a rise in the compression rate while pel-
leting rice straw at variable compression rates (44.5–75.5
mm/min) using a single pellet unit (Hu et al. 2013). Wu
et al. (2010) noticed a similar observation for extruder die
speed. The high speed of the extruder die produced pellets
13

with a smaller height, thus improving the pellet durability.
A lower extruder die size results in an extremely durable
pellet. A study found that pellet density increased by 6%
when extruder die diameter decreased from 15 mm to 12 mm
(Pradhan et al. 2018a). Thrän et al. (2016) reported the high-
est durability of pellets produced using 6 mm of extruder die
diameter compared to those obtained from 8 mm diameter.
The durability of a densified material is also influenced by
its shape. For example, sharp edge materials have poor abra-
sion resistance compared to those with a rounded curved
edge regardless of other densification conditions.
Due to an increase in shear stress, a higher length-to-
diameter ratio equates to the greater durability of the pellet.
However, a high shear force could cause the pellet mill to
clog (Pradhan et al. 2018b; Nielsen et al. 2020). Moreo-
ver, extruder die choking is found frequently in the case
of smaller dies at a specific feed moisture percentage and
milling size despite their lower throughput capability. The
pelletizing pressure increases as the extruder die length
increases, but the pressure reduces as the diameter of the
extruder die increases (Tumuluru et al. 2011). Thus, the size
of the extruder die and the matrix’s press channels have a
significant impact on the pressure required to densify bio-
mass through the matrix.
Pelletized materials typically exit the pelletizer at a tem-
perature between 60 °C and 95 °C and moisture contents of
12–18 wt% although the ideal moisture content is typically
5–8 wt% (Carroll and Finnan 2012). Therefore, a cooling
step is required before storage or transportation as pellets
may lose their quality and result in post-transport and stor-
age heating, combustion and caking if they are not properly
chilled and dried. Moreover, rapid cooling of pellets may
result in the brittleness of the exterior layer due to fast cool-
ing, while the inner layer could remain warm, thus causing
stress in the material and the creation of cracks in the outer
layer.
Pretreatment technologies for biomass
pelletization
Steam explosion
Steam explosion is a common lignocellulosic biomass pre-
treatment method performed at 200–260 °C for 5–10 min
under rapid decompression with the purpose of lignin acti-
vation by using high pressurized steam of 1–3 MPa. Since
it increases cellulose accessibility, it is widely used for
bioethanol production. However, it has also been used for the
production of solid fuel pellets during the steam explosion,
which causes plant cell walls to explode exposing cellulose
fibers and depolymerized lignin to be more accessible for
densification. This can boost the binding mechanism without
13
Environmental Chemistry Letters
increasing pelletizing pressures (Pradhan et al. 2018b). In
addition to solubilizing hemicellulose, biomass is subjected
to explosive decompression, which lowers its particle size.
The need for biomass grinding in traditional biomass pelleti-
zation methods is reduced as a result of this size reduction
(Tumuluru et al. 2010).
Liu et al. (2013) observed that stream treatment reduced
the particle size of biomass that is directly used in pelletiza-
tion without performing the grinding test. The potential for
a steam explosion to improve pellet durability has been stud-
ied extensively (Adapa et al. 2010; Lam et al. 2011). A prior
study found that the severity of a steam explosion increased
the compression energy of Douglas fir (Adapa et al. 2010;
Lam et al. 2011). However, the energy requirement for pel-
letization of biomass was reduced by 13% for steam pre-
treated biomass conducted at 180 °C and 1 MPa (Adapa
et al. 2013). It has been reported that steam explosion of
biomass produces pellets with low ash content with higher
mechanical strength, which enlightens the combustion prop-
erties of produced pellets (Kumar Biswas et al. 2014).
Mckechnie et al. (2016) also observed that steam-treated
pellets significantly reduced greenhouse gas emissions com-
pared to coal. The unit density of pellet obtained from steam-
treated biomass is usually higher than the untreated biomass
pellet because lignin and sugars have a stronger binding role
between pretreated particles (Chang et al. 2012). Lam et al.
(2015) found that pseudo-lignin triggered by steam explo-
sion pretreatment improved the softwood fibers’ binding
ability to form durable pellets. They also stated that steam
pretreatment enhanced the pellet quality by improving
Meyer hardness and mechanical strength, and reported that
the duration of treatment improves dimensional stability and
elasticity. Biswas et al. (2011) conducted steam pretreatment
for wood pellet production from Salix and noticed that pellet
properties such as density, impact resistance and abrasion
resistance as well as higher heating value augmented after
pretreatment, while ash content, especially alkali metals,
reduced to a greater extent.
Kumar et al. (2012) concluded that steam-treated residue
yielded a high-density wood pellet even at low pressure of
72 MPa for Salix while conducting steam pretreatment at
190–200 °C for 5 min with ­SO2 impregnation. Tang et al.
(2018) investigated five steam pretreatments such as auto-
hydrolysis, deacetylation, acidic sulfonation, ­SO2 catalysis
and neutral sulfonation on the quality of poplar pellet. The
results showed that the autocatalytic steam explosion pro-
cess produced more durable pellets with high calorific value
compared to others.
Environmental Chemistry Letters
Torrefaction
Torrefaction is an extensively used thermal pretreatment of
lignocellulosic biomass performed at 200–300 °C under an
oxygen-deficient environment with the purpose of solid fuel
production with enhanced energy density (Tang et al. 2018;
Sarker et al. 2021a, b). Moreover, grindability and homoge-
neity remarkably increased due to torrefaction pretreatment
of biomass. Torrefaction significantly removes moisture and
volatile matter while degrading hemicellulose content, thus
improving the hydrophobicity of torrefied biomass. This is
important for long-term storage and long-distance transpor-
tation. Several researchers have examined the combined tor-
refaction and pelletization method for more than a decade
(Kang et al. 2019). During torrefaction, around 30% of the
mass can be lost as moisture and volatile matter, but torrefied
biomass may contain up to 90% of its initial energy content.
Chen et al. (2022a, b) observed that density, hydrophobic-
ity, energy content and Meyer hardness increased for torre-
fied biomass pellets produced from rice husk and rice straw.
Yang et al. (2019) conducted a synchronized torrefaction and
pelleting of corn stover and Big bluestem using a single pel-
let unit and perceived that the synchronized torrefaction and
pelleting constantly produced pellets with amended physi-
cal, thermochemical and hygroscopic properties. They also
concluded that the synchronized torrefaction and pelleting
techniques were promising for producing more durable and
dense torrefied pellets. Pellet durability and bulk density
were positively prejudiced by the torrefaction temperature of
biomass (Rudolfsson et al. 2017). Higher torrefaction tem-
peratures resulted in greater power consumption during pel-
letization owing to increased friction in the press channels.
It has been reported that pelletization of torrefied biomass is
comparatively more difficult than raw biomass as it requires
high pressure and high temperature as well as external addi-
tives to improve the interparticle bonding.
In a study by Sarker et al. (2022b), the durability, density
and higher heating value of torrefied pellets were greater
than raw pellets from canola residue. However, the addi-
tion of bio-based binders such as lignin, bio-oil and mustard
meal further improved the pellet quality of torrefied canola
residue, while energy densities obtained were 15.6, 19.4 and
21.2 GJ/m3 for raw, torrefied pellets and torrefied pellets
with bio-additives, respectively. Dai et al. (2019) reported
the addition of biomass gasification residue to boost the ten-
sile strength of the pellet while investigating the effects of
different bio-based additives such as lignin, starch and poly-
vinyl alcohol with biomass gasification residues on pellet
properties obtained from carbonized sawdust.
Torrefaction can also be used as a post-treatment method
for fuel pellets. It has gained attention recently due to
several problems associated with the pelletization of tor-
refied biomass. It has been mentioned that torrefaction of
post-treatment of biomass pellets can result in pellets with
enhanced calorific value and improved hydrophobicity but
reduced density and mechanical strength, which may cre-
ate dust and fines during transportation and handling. In
contrast, torrefaction of biomass requires additives for pel-
letization with desirable quality. Therefore, the torrefaction
operating conditions can be optimized to produce pellets
with the optimal combination of qualities to meet mechani-
cal and thermal requirements. For example, the mass loss
caused by the torrefaction process can be compensated by
increasing the materials’ heating value.
Siyal et al. (2020) conducted torrefaction of sawdust and
furfural pellets at various temperature ranges and time of
200–300 °C and 15–120 min, respectively. They reported
that both hydrophobicity and heating value increase with
the rise in torrefaction severity. However, the highest energy
density was found at 300 °C for 120 min. Peng et al. (2015b)
concluded that biomass requires torrefaction before com-
pression to produce durable pellets with a high volumetric
energy density and hydrophobicity. On the contrary, Peng
et al. (2015a) reported that the quality of torrefied pellets
was relatively poor than the pellets produced from torrefied
sawdust. Brachi et al. (2019) conducted torrefaction of pel-
lets produced from woody and non-woody biomass under
oxygen and nitrogen as the carrier gases in a fluidized bed
reactor. The results showed that the mechanical hardness
and durability of pellets produced from woody biomass were
affected negatively by torrefaction severity. In the case of
olive pomace pellets, the durability and hardness slightly
increased with torrefaction. The authors also mentioned that
oxidative torrefaction showed higher pellet quality compared
to torrefaction performed under an inert atmosphere.
Manouchehrinejad and Mani (2018) carried out torrefac-
tion of two commercial wood pellets at 230–290 °C for 30
min and concluded that 270 °C provided the highest volu-
metric energy density and heating value. The increased tor-
refaction temperature enhanced the hydrophobicity of pellet
but decreased hardness, density and durability making torre-
fied pellets more prone to breakage and fine generation dur-
ing handling, transportation and storage. Similar behavior in
calorific value was also observed by other researchers (Chen
et al. 2016b). The calorific value of pellets increased by 17%
after torrefaction compared to raw pellets, while hydropho-
bicity increased by 1.6 times, and the combustion behavior
of torrefied pellets showed a 5% increment in combustion
efficiency (Isemin et al. 2017).
The porosity of pellets significantly increased after tor-
refaction resulting in a decrease in mechanical strength,
which may be attributed due to the removal of volatiles
during torrefaction (Isemin et al. 2017; Azargohar et al.
2019b). However, Ghiasi et al. (2014) compared two process
schemes such as scheme I (torrefaction before pelletization)
and scheme II (torrefaction after pelletization) in terms of
13

pellet quality and energy efficiency. In comparison to pellets
produced through scheme I, pellets generated by scheme II
demonstrated lower water adsorption and a 6% greater calo-
rific value. They mentioned that scheme I required higher
compression force and an external binder to pelletize bio-
mass. They concluded that scheme II is more promising for
the production of torrefied pellets compared to scheme I. In
another study, torrefaction was compared both as pretreat-
ment and post-treatment based on pellet quality (Sarker et al.
2022a). The authors reported that there was not much dif-
ference in pellet durability and calorific value but the bulk
density of pellets significantly decreased when torrefaction
was used as a post-treatment method.
Hydrothermal carbonization
Hydrothermal carbonization is one of the promising hydro-
thermal pretreatment processes for converting biomass with
a high moisture content into solid biofuels (González-Arias
et al. 2022). The process requires moderate temperatures
of 180–350 °C and comparatively higher pressures of 2–10
MPa. Biochar produced at low temperatures (less than
300 °C) typically has carbonyl and carboxyl structures on
its surface with micropores and mesopores, thus proving
excellent reactivity. In contrast, biochar produced at high-
temperature hydrothermal carbonization (more than 300 °C)
derived biochar has more carbon even with graphitic struc-
tures. Furthermore, hydrothermal pretreatment lowers the
ash content of biochar by moderately dissolving ash in
water. Thus, the ash-related challenges during combustion
are reduced.
Murillo et al. (2021) investigated the combustion behav-
ior of fuel pellets produced from hydrothermally carbon-
ized biomass in a household pellet stove and observed that
hydrochar pellets significantly reduced the emissions of CO,
­NOx and particulate matter compared to raw biomass pellets.
Hydrochar is a carbonized material obtained from hydro-
thermal carbonization, supercritical water gasification and
hydrothermal liquefaction (Kang et al. 2020, 2022; Masoumi
et al. 2021; Jha et al. 2022). Mittapalli et al. (2021) carried
out hydrothermal carbonization of anaerobic granular sludge
followed by the production of hydrochar and further pel-
letized with yard wastes. Their results show that hydrochar
pellets enhanced the compressive strength by 27% compared
to pellets produced from raw biomass. Furthermore, hydro-
char pellets showed greater calorific value, high hydropho-
bicity and improved combustion properties.
Moreira et al. (2021) pelletized spent coffee ground with
biochar derived from hydrothermal carbonization of food
waste. They noticed that the addition of biochar and ash
from hydrothermal carbonization of food waste acted as a
lubricant and additive during pelletization and enhanced
pellet durability. Sharma and Dubey (2020a) investigated
13
Environmental Chemistry Letters
the effects of temperature and reaction time on hydrochar
pellets from municipal yard waste. They reported that the
tensile strength of the pellets augmented from 1.5 MPa to
4.8 MPa with the rise in severity factor, which was attributed
to a stronger interparticle bonding as lignin from hydrochar
softens at higher temperature and acted as a natural binder
during pelletization. In addition, energy density, impact
resistance and hydrophobicity are significantly influenced
by the severity factors. Bonding between hydrochar pellets
is much strong than raw biomass particles.
Sharma and Dubey (2020b) compared the pelletization
behavior and properties of pellets produced from yard waste
and food waste hydrochar. They noticed that hydrochar pel-
lets from yard waste were stronger than those from food
waste due to the high lignin content in yard waste. Further-
more, they concluded that the pellets from yard waste and
food waste hydrochar pellets offered attractive fuel quality.
Another study reported that hydrochar pellets released more
aldehydes and ketones due to unsaturated fatty acid com-
pounds in the char (Li et al. 2018). Zaini et al. (2017) pel-
letized hydrochar and washed hydrochar from empty fruit
bunches and found that washed hydrochar pellets exhibited
higher durability and mechanical strength than those from
raw empty fruit bunches and hydrochar alone. This indi-
cates that hydrothermal carbonization is a promising solu-
tion for pelletizing high-moisture biomass in controlled
environments.
Biological pretreatment
Biological pretreatment of lignocellulosic biomass refers to
the use of fungi, bacteria and other microorganisms in a
controlled environment to disintegrate lignocellulosic com-
pounds and make the carbohydrates more accessible (Sarkar
et al. 2012; Sindhu et al. 2016; Sharma et al. 2019). It also
causes denaturation of refractory biomass, which improves
particle interlocking capacity and flowability at the time of
pelletization. Biological pretreatment is being investigated
for densification of biomass as a simpler, safer, less energy-
intensive and cost-effective method with fewer environmen-
tal implications than thermochemical pretreatments (Sharma
et al. 2019).
Gao et al. (2016) investigated solid-state fermentation to
improve the quality of pellets produced from barley straw.
Another study also investigated the quality of wheat straw
pellets using biological pretreatment via solid-state fermen-
tation by using three different fungal strains, namely Tram-
etes versicolor m4D, Trametes versicolor 52J and Phan-
erochaete chrysosporium (Gao et al. 2017). Their findings
revealed that after processing, the interlocking between fib-
ers became comparatively loose, thus improving the pel-
lets’ compressibility. Another study found that treating
sawdust biologically via solid-state fermentation improved
Environmental Chemistry Letters
hydrophobicity, Meyer hardness and density of pellets as
compared to those made from raw sawdust (Guo et al. 2015).
However, biological processing is typically time-intensive
compared to thermochemical treatments. In addition, more
research is required in this area to provide insights into the
underlying mechanisms of the biological decomposition of
biomass and its contribution to the final pellet quality.
Hydrophobic coating
Hydrophobicity or resistance to moisture is an essential
aspect of fuel pellets. It is recognized that pellets made from
agricultural and forest residues swell and disintegrate when
exposed to moisture, thus creating a significant issue dur-
ing bulk transportation and storage. Moreover, an increase
in moisture also encourages microbial activity resulting in
a decrease in pellet quality. Therefore, to make the pellet
resistant to water, a coating can be applied. Craven et al.
(2015) studied to create moisture-stable wood pellets by
introducing a hydrophobic coating. Paraffin oil, mineral
oil, castor oil and linseed oil are used to treat pellets. Thus,
this treatment reduces the creation of airborne particles
and a rise in the energy density of wood pellets, amplifying
calorific value up to 1.2 MJ/kg. Kaliyan and Morey (2010)
reported a similar observation that the addition of lignin to
the outer surfaces of biomass samples improved the water
resistance of various biomass pellets.
Tilay et al. (2015) used a coating on freshly prepared
canola meal pellets using a coating agent, especially 4%
dissolved in 85% isopropanol followed by drying in an oven
at 100 °C for 30 s to enhance long storage. Coated canola
meal pellets were found to preserve their native pellet qual-
ity for up to eight weeks, while the durability and hardness
of uncoated pellets significantly dropped. The swift drop in
moisture content from 8 to 0.7 wt% was due to the residual
isopropyl alcohol evaporation during storage, which removes
the bound moisture from the pellets. The moisture content
of control pellets without coating increased from 6.8 wt% to
7.9 wt%, thus making them less durable. The coated pellets
have demonstrated better stability in an ambient environment
compared to the controlled pellets. Thus, hydrophobic pellet
coating is one of the options for producing stronger, more
durable and moisture-resistant pellets.
Additives for pelletization
Additives or binders are added to biomass during the prepa-
ration of pellet formulation. Additives enhance the binding
mechanism of pellets, thereby promoting their mechanical
strength and durability. Besides, additives also help to lower
the energy consumption during densification to improve
combustion properties and reduce the wear and tear of the
pellet die. These can aid in lowering the net greenhouse gas
emissions and maintenance costs. Current technical criteria
suggest that additives should not proportionate more than
2% of the total pellet weight for better quality.
Though the application of additives in pellet formula-
tion is firmly limited, different types and proportions of
additives have been used to investigate their effects on
pellet quality. The additives can be from a wide range of
organic and inorganic sources including raw and treated
biomasses, municipal solid waste, forest residues, byprod-
ucts from different processes and industrial wastes. How-
ever, understanding the attributes of the additives to be
employed in a densification process is critical as additives
may differ in features from biomass and may affect the
binding mechanism. Therefore, when deciding whether or
not to use a binder, it is important to consider the environ-
mental effects and the impact that the binder will have on
the long-term viability of the pellets.
As an additive, binders perform like adhesive resins
used in particle and fiberboard manufacturing. A proper
quantity of binder can enhance the mechanical property,
energy density as well as combustion properties by reduc-
ing particulate matter emissions. Lignocellulosic biomass
contains some natural binding agents such as lignin, fat,
starch, protein and carbohydrates, which are activated
at high temperatures and pressures during pelletization.
Some feedstocks contain too low-natural binding agents
because of their different sources or pretreatments since
they cannot be activated to allow efficient binding under
the given densification conditions. Furthermore, because
of the lack of natural binding chemicals, the accumula-
tion of a secondary feedstock like charcoal or another
substance may result in inadequate binding. Hence, exter-
nal binders are needed to overcome this issue. There are
various kinds of additives varying in their state and shape
to initiate and promote particular interactions through a
chemical reaction. Several binders have been investigated
so far but the extent to which they operate remains an
intriguing topic. Table 1 shows different additives used
with various biomass at variable pelletization conditions.
Table 2 depicts different lubricants and emissions used
during pelletization.
Lignin
Lignin is an essential component of lignocellulosic biomass
rendering structural integrity to plant cell walls (Nanda et al.
2014; Fougere et al. 2016). One of the widely used additives
for the pelletization of wood and agricultural residue is lignin/
kraft lignin, a byproduct of the pulp and paper industry. It
is extracted from black liquor, which contains alkali-soluble
lignin with a significantly different structure than natural
13

Table 1  Additives as binders used for pelletization of biomass
Additive
13
Algae (Rhizoclonium spp.)
Ca-Mg-lignosulphonate
Cassava stem and potato starch
Coal tar residue
Corn starch and molasses
Cow dung and molasses
Crude glycerin and paraffin
Amount (wt%) Feedstocks Pelleting conditions Main observations References
10–90 Miscanthus straw Compression force: 1000 N Algal biomass enhanced the Thapa et al. (2015)
Relaxation time: 5 s binding mechanism of Mis-
canthus pellets, which remark-
ably increased the compression
strength without affecting the
calorific value of pellets
1 and 2 Poplar and pine sawdust Temperature: 93 °C The addition of 2% lignosulpho- Monedero et al. (2015)
nate revealed the highest pellet
durability, bulk density and parti-
cle density
0.5–5 Scots pine and Norwegian spruce – The additives amplified the dura- Larsson et al. (2015)
sawdust bility of pellets and diminished
the generation of fines and CO
emission
0–40 Sawdust, wheat straw and bamboo Relaxation time: 10 s Abrasive resistance increased from Cheng et al. (2018)
Temperature: 80 °C 10.6–69% to 96–98% for wheat
Pressure: 100 MPa straw, sawdust and bamboo pel-
lets. The calorific value of pellets
also increased by 21–26%
0.8–2.8 and 0.5–1.8 Norway spruce and Scotch pine Relaxation time: 10 s The addition of additives made Ståhl et al. (2016)
Temperature: 116 °C the pelletization process more
Pressure: 10.8 MPa efficient. However, ­CO2 emis-
sions increased with the amount
of additives added
0–100 Wheat straw and rice husk – Pellets with 98% durability and Iftikhar et al. (2019)
the calorific value of 19.1 MJ/kg
were obtained with 8.5% of cow
dung. Cow dung contains a high
amount of lignin which helped
in enhancing pellet properties.
Effects of molasses were insig-
nificant on pellet strength and
durability
1–10 Rice straw Relaxation time: 60 s The addition of 4% paraffin Xia et al. (2019)
Temperature: 120 °C reduced the energy consump-
Pressure: 60 MPa tion of the pelletization process
for hydrothermally carbonized
biomass by 37.2%. This also
augmented the calorific value of
pellets by 68% and pellet density
by 7.7%, while decreasing tensile
strength by 4.3%
Environmental Chemistry Letters
 Table 1  (continued)
Additive
Crude glycerol
Dairy powder waste
Dolomite and lime
Glycerol
Grape pomace, olive pomace,
almond shell, olive stone, cocoa
shell and Miscanthus
Lignin and amino acid
Lignin, calcium hydroxide, starch,
and sodium hydroxide
Lignin, L-proline and nipecotic
acid
13
Amount (wt%) Feedstocks Pelleting conditions Main observations References
10–15 Sugarcane bagasse, coffee husk Temperature: 70 °C With an increase in binder Marrugo et al. (2019)
and rick husk quantity, the calorific value of
pellets increased but water resist-
ance and pellet density slightly
decreased. Crude glycerol also
acted as a lubricant thus reducing
the degree of compaction
Environmental Chemistry Letters
0–20 Food waste compost – The dairy powder contained more Chew et al. (2018)
lactose, which significantly
improved the production rate,
compressive strength and density
of the pellets. The addition of
lactose provided more solid
bridges by crystallization leading
to stronger bonds within the
pellets
2 Wood chips – The addition of lime and or Kafle et al. (2017)
dolomite increased the physical
and mechanical properties of the
pellets while reducing the tar
content
10 and 40 Sawdust – The highest durability of the pel- Bartocci et al. (2018)
lets was obtained at 20% glycerol
50 Pine sawdust and torrefied pine Compression force: 15 kN Lignin-enriched solid additives García et al. (2018)
sawdust such as grape pomace improved
the binding mechanism of both
raw and torrefied pine sawdust
3–17 and 4–10 Raw and microwave torrefied oat Compression force: 4000 N Lignin improved the calorific value Abedi and Dalai (2017)
hull Relaxation time: 60 s and ash content of the pellets
Temperature: 100 °C
5–20 Rice husk biochar Compression force: 30 kN Pellets prepared with lignin and Hu et al. (2015)
Relaxation time: 180 s Ca(OH)2 showed the high-
est mechanical strength and
improved the combustion proper-
ties while reducing moisture
absorption and energy consump-
tion during compression
2–6 Canola hull Compression force: 3500 N Desired quality pellets were Azargohar et al. (2019a)
Relaxation time: 35 s obtained when L-proline was
Temperature: 100 °C used

Table 1  (continued)
Additive
13
Lignin, sawdust and mustard meal
Lignin, starch, polyvinyl alcohol
and biomass gasification residue
Linear low-density polyethylene
extracted from municipal solid
waste
Microalgae, biosolids and starch
Molasses, fructose, glucose,
maltodextrin, sucrose and ligno-
sulfonate
Papermaking sludge
Peptides from hydrolyzed specified 0–3
risk materials with polyami-
doamine epichlorohydrin resin
Amount (wt%) Feedstocks Pelleting conditions Main observations References
10 Torrefied canola hull Compression force: 3500 N The addition of 10% lignin and Sarker et al. (2022b)
Temperature: 100 °C mustard meal upgraded the pellet
Relaxation time: 35 s quality. The effects of sawdust
addition were insignificant
4.9–12.9, 0–16 Sawdust biochar Temperature: 100 °C Polyvinyl alcohol showed better Dai et al. (2019)
Pressure: 100 MPa bonding and hydrophobicity than
starch and lignin. 4.3% addition
of biomass gasification residue in
polyvinyl alcohol improved the
strength from 26.3 to 35.3 N/mm
1–10 Torrefied wheat straw and barley Compression force: 4 kN The addition of 10% linear low Emadi et al. (2017)
straw Temperature: 150 °C density polyethylene to torrefied
biomass pellets increased tensile
strength by 280% and 253% for
wheat straw and barley straw
pellets, respectively. It also
increased the calorific value of
pellets and reduced their ash
content
6 Corn cobs, rice husk and sugar- Pressure: 19–31 MPa Microalgae improved the calorific Muazu and Stegemann (2017)
cane bagasse value, durability and stability of
pellets
4–12 Wheat straw and spruce wood Compression force: 4000 N Molasses and fructose were the Soleimani et al. (2017)
shavings Relaxation time: 60 s best binders for wheat straw and
Temperature: 90 °C spruce wood shavings, respec-
tively exhibiting desirable solid
fuel properties
0–40 Wheat straw Temperature: 95 °C With a rise in glycerol content, the Matúš et al. (2018)
durability of pellets increased
but the calorific value decreased
significantly
Torrefied spruce and fir sawdust Temperature: 80–85 °C The addition of 3% polyamidoam- Adhikari et al. (2019)
ine epichlorohydrin resin sig-
nificantly improved the calorific
value, durability and bulk density
of torrefied biomass pellets
Environmental Chemistry Letters
 Table 1  (continued)
Additive
Potato pulp
Rapeseed flour, bark, lignin pow-
der, coffee meal and pine cones
Raw sawdust, starch and lignin
Sodium carboxymethyl cellulose
13
Amount (wt%) Feedstocks Pelleting conditions Main observations References
10–30 Buckwheat hulls – Energy consumption decreased by Obidziński et al. (2016)
66% when potato pulp addi-
tion increased from 10 to 30%.
The density and durability of
pellets slightly decreased with
the amount of additives. A 20%
additives amount was optimum
Environmental Chemistry Letters
for high-quality pellets
2–10 Tulip tree and Larch Relaxation time: 180 s Lignin, rapeseed flour and coffee Ahn et al. (2014)
Pressure: 1.5 MPa meal enhanced the durability and
calorific value of the pellets from
both the feedstocks
5–30 Torrefied pine sawdust Relaxation time: 60 s The addition of raw sawdust Strydom et al. (2018)
Temperature: 70 °C enhanced the pellet density and
Pressure: 125 MPa durability. Sawdust was recom-
mended as a better binder than
starch and lignin due to its low
cost and abundance in avail-
ability
5 cotton stalk, corn stalk, rice husk, Relaxation time: 180 s The addition of carboxymethyl Zhu et al. (2018)
camphorwood Temperature: 105 °C cellulose significantly increased
Pressure: 120 MPa the emission of particulate mat-
ter while increasing the pellet
quality


Table 2  Additives as lubricants used to reduce emissions during pelletization of biomass

Additive Role Amount (wt%) Feedstocks Pelleting conditions Main observations Reference

13
Aluminosilicate Emission reduction 5–25 Wood pellet, olive cake, soft- – The quantity of potassium Clery et al. (2018)
wood and wheat straw released during char oxida-
tion and ash cooking was
reduced by adding alu-
minosilicate. The amount
of additives needed was
proportional to the amount
of potassium present in the
biomass
Aluminosilicate base additives Emission reduction 1.5 and 2 Wood pellets – Potassium chloride reacted Paneru et al. (2016)
with aluminosilicate addi-
tives to reduce chlorine
levels in fly ash and deposits,
thus lowering the risk of cor-
rosion at high temperatures
Bio-oil Binder and lubricant 7.5 and 15 Barley straw, oat hull and – The addition of 15% bio- Sarker et al. (2021a, b)
canola hull oil resulted in the highest
durability, energy density
and mechanical strength of
the pellets
Coal tar residue Emission reduction 30 Sawdust, bamboo and wheat Relaxation time: 10 s The addition of coal tar residue Si et al. (2017)
straw Pressure: 100 MPa in biomass pellets reduced
the emissions of S ­ O2, NO,
polyaromatic hydrocarbons
as well as polychlorinated
dibenzo-p-dioxins and poly-
chlorinated dibenzo-p-furans
compared to those from
direct combustion of coal tar
residue
Crude glycerol, pure glycerol Lubricant Wheat straw and spruce wood Compression force: 4000 N Pure glycerol acted as a binder Soleimani et al. (2017)
and canola oil shavings Relaxation time: 60 s rather than lubricant, while
Temperature: 90 °C canola oil performed best as
a lubricant
Glycerol Lubricant 10–30 Raw and torrefied pine sawdust Compression force: 15 kN Glycerol as a lubricant García et al. (2018)
increased the calorific value
of pellets and improved their
lubricating characteristics,
particularly in torrefied
biomass. However, a higher
amount of glycerol reduced
the binding ability, durability
and density of the pellets
Environmental Chemistry Letters
 Table 2  (continued)
Additive
Glycine and crude glycerol
Kaolin, Diatomite, carboxy-
methyl cellulose, calcium
hydroxide and Bentonite
Pyrolysis oil
Rapeseed oil
Sunflower oil
13
Role Amount (wt%) Feedstocks Pelleting conditions Main observations Reference
Lubricant 4–10 Canola hull Compression force: 3500 N Crude glycerol decreased Azargohar et al. (2019a)
Relaxation time: 35 s energy consumption during
Temperature: 100 °C biomass pelletization. The
tensile strength of the pel-
lets was reduced with pure
glycerol
Emission reduction 5 Cotton stalk Relaxation time: 180 s Diatomite effectively reduced Yang et al. (2018)
Environmental Chemistry Letters
Temperature: 50–300 °C the particulate matter emis-
Pressure: 120 MPa sion. However, composite
additives such as diatomite
with carboxymethyl cellulose
also improved the reduction
of particulate matter
Lubricant 15 Torrefied canola hull Compression force: 3500 N Pyrolysis oil resulted in a Sarker et al. (2022b)
Relaxation time: 35 s smoother extrusion and
Temperature: 100 °C improved hydrophobicity and
calorific value of the pellets
Lubricant 2 Wood chips Relaxation time: 5 s The addition of 2% rapeseed Shang et al. (2014)
Temperature: 125–190 °C oil reduced the friction
Pressure: 300 MPa by 50% during extrusion
thus lowering the energy
consumption and improving
pellet properties
Lubricant 1–3 Oat hull Compression force: 4000 N Sunflower oil lowered the Abedi and Dalai (2017)
Relaxation time: 60 s energy consumption by
reducing friction during
extrusion and increased the
calorific value of the pellets.
However, pellet density and
strength slightly decreased

lignin. Kraft lignin has a molecular weight of 10,000–50,000
g/mol and an anionic charge density of 0.1–0.9 meq/g (Anu-
kam et  al. 2021). Moreover, it contains some functional
groups in its highly branched structure, which have been
ascribed to its ability to be utilized as an additive in the pelleti-
zation of lignocellulosic biomass. The addition of 15% alkali
lignin to fiberboards significantly improved the mechanical
properties (Mancera et al. 2011). Hu et al. (2015) discovered
that adding 10% alkali lignin to wood pellets increased their
durability significantly. The addition of 6 wt% of alkali lignin
increased the durability of canola hull pellets by 26% (Azargo-
har et al. 2019a). Lignin is also found in enhancing oat hull
pellet quality (Abedi and Dalai 2017).
Lignosulfonate
Lignosulfonate, a by-product of the pulping process in pulp
and paper industries, is extensively used as an effective bind-
ing agent for pelleting lignocellulosic biomass. Lignosulpho-
nate, usually derived from sulfonated lignin, is easily soluble
in water and anionic solvent because the benzylic carbon
atoms in its structure are connected by sulfonic groups.
The majority of lignosulfonates are made from spent sulfite
liquor, which mostly comprises both organic and inorganic
compounds derived from lignin including residual salts from
the pulping process, 7–8 wt% lignosulfonates and approxi-
mate 4 wt% sugars (Restolho et al. 2009; Saeed et al. 2011).
Lignosulfonate is an excellent addition to biomass pel-
leting because of its surface-active properties (Reza et al.
2012). Lignosulfonates are made up of sulfonated lignin
fragments of various molecular sizes such as inorganic salts,
sugar monomers and minor amounts of extractives. Though
lignosulfonate helps in the binding of biomass during pel-
letization, its usage as an additive is limited because of hav-
ing high inorganic salt content. It may result in high ash
deposition during combustion. It has been mentioned that
lignosulfonate content higher than 34 wt% in biomass may
affect the pellet properties, especially durability negatively.
Thus, 1–3 wt% of lignosulfonate is recommended for pellet
production from biomass (Crawford et al. 2016; Azargo-
har et al. 2018). Lignosulfonate significantly upsurges the
density, tensile strength and higher heating value of pellets
while reducing the specific energy consumption (Lu et al.
2014). The use of lignosulfonate can also increase the sulfur
content of produced pellets (Obernberger and Thek 2004).
Starch
Starch is another popular binding agent, which consists of
polysaccharides such as amylose and amylopectin. While
α-1,4 glycosidic bonds responsible for the formation of
unbranched chains are found in amylose, α-1,6 glycosidic
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Environmental Chemistry Letters
bonds are found in amylopectin. Hydrogen bonds in starch
support helical conformation, which provides vicinal
hydrophobic surfaces conducive to bonding. The complete
chemical structure of starch consists of two monomer units
including amylopectin and amylose. The chemical structures
of that unit influence the ease with which water penetrates
the starch granules. The formation of concentric regions of
alternating amorphous and crystalline structures is due to
amylopectin content. When starch is used as an additive in
biomass densification, the chemical structures provide a bal-
ance of mechanical stability and durability of the pellets.
The addition of starch enhances the bonding resulting in
higher durability and pellet strength while reducing abra-
sion. The properties of starch are extremely uneven making
it tough to precisely estimate its impacts in the densification
process. A study used cornstarch for pelleting sawdust from
different woody biomass and reported that energy consump-
tion decreased due to the addition of starch additives, while
­CO2 emission slightly increased (Ståhl et al. 2016). The
addition of starch also increases the density and strength of
pellets produced from torrefied biomass (Peng et al. 2015a).
Spent sulfite liquor
Spent sulfite liquor or brown liquor is a carbohydrate-rich
lignosulfonate leftover from the pulping process. The molec-
ular structure of spent sulfite liquor is comparable to that of
lignosulfonate but with changes in molecular weight and
characteristics. Spent sulfite liquor can be obtained from the
delignification of wood chips in the presence of a sulfur-
ous acid or bisulfite solution at high temperatures and pres-
sures. Spent sulfite liquor is a suitable additive for enlighten-
ing interparticle bonding and due to its high viscosity and
adhesive nature allows substantial intermolecular forces of
attraction when employed as an additive during pelletiza-
tion. Spent sulfite liquor remarkably decreases the energy
consumption but increases pellet density for biomass pel-
lets (Ståhl et al. 2016). Due to the potential in enhancing
pellet properties and cutting down the energy consumption,
spent sulfite liquor can be used for densifying lignocellulosic
biomass.
Bio‑oil
Bio-oil is a co-product obtained from pyrolysis of bio-
mass under inert atmospheres as a result of thermal crack-
ing of biomass, devolatilizaton and condensation of vola-
tile hydrocarbon vapors (Nanda et al. 2016). Pyrolysis or
liquefaction-derived bio-oil is recently being investigated
as a binding and/or lubricating agent during the densifica-
tion of biomass. Bio-oil from pyrolysis or liquefaction of
biomass mostly contains tar having a high viscosity, which
Environmental Chemistry Letters
influences interparticle bonding (Suresh et al. 2021). Kang
et al. (2018a) compared various pellets produced from apple
tree branches with bio-oil and alkali lignin. They noticed
that pellets produced with bio-oil had higher density, hydro-
phobicity, strength and higher heating value compared to
that produced with alkali lignin. Another study compared
the effects of two different bio-oils obtained from the apple
tree branch and Eucommia ulmoides Oliver tree for pelleti-
zation of biochar (Kang et al. 2018b). The authors reported
that bio-oil obtained from the apple tree branches was the
optimal binder for improving biochar pellet quality. Both
binding and lubricating effects were found for softwood-
derived pyrolysis oil for pelletization of agricultural residue
(Sarker et al. 2021a, b). Bio-oil is also found to reduce the
energy consumption of the densification process by lowering
the extruder die friction (Sarker et al. 2022b).
Waste plastics
Plastic pollution is a major environmental challenge today
(Nanda and Berruti, 2021a, b; Nanda et al. 2021; Yang et al.
2022). Plastic waste has recently gained attention as an effec-
tive binder for pelletization and as a co-feedstock for thermo-
chemical conversion (Nanda et al. 2022). Using plastic waste
as a binder not only minimizes pollution but will also reduce
greenhouse gas emissions that would otherwise be caused by
the recycling or incineration of plastics. Peng et al. (2021)
used different plastics including pure recycled polyethylene
bottles and bags, polyethylene resins, recycled polyethylene
terephthalate bottles and recycled polypropylene bottles for
pelletizing pine woodchips. They compared the pellet qual-
ity with those prepared from widely known additives such as
lignin and corn starch. Their results showed that pellets pre-
pared from pyrolyzed biochar at 330 °C with plastics as the
binder had higher hydrophobicity, higher energy density and
greater hardness compared to those from raw biomass pellets
and pellets made with starch and lignin. The use of a linear
low-density polyethylene binder enhanced the pellet density
while lowering the ash content (Emadi et al. 2017). A study
reported that the tensile strength of barley straw and wheat
straw pellets amplified by 253% and 280%, respectively due
to their higher tensile strength of 18 MPa and capacity to
form strong interlocking of torrefied biomass particles (Sat-
pathy et al. 2014).
Characterization of biomass pellets
Table  3 represents the different physical, chemical and
mechanical properties of biomass pellets with their com-
mon characterization or measurement techniques.
Density
Density is the most important parameter to consider in the
compaction of biomass particles under pressure during pel-
letization. Bulk density, particle or unit density and tapped
density evaluate the density of pulverized and pelletized
biomass. Both tapped and bulk density have remarkable
effects on combustion behavior as well as storage and
transportation. Bulk density is usually determined by pyc-
nometer or displacement methods in which pellets or pul-
verized biomass are progressively poured into a container
of known volume until physical saturation. The bulk den-
sity is calculated as the ratio of the mass of the biomass
over the volume of the container. Unit density, also known
as true density, is the apparent, real, absolute and skeletal
density of a single pellet determined by dividing the mass
by volume, while volume can be calculated by measuring
the dimension of pellets. Unit density is usually measured
after pellet production.
After pelletization, the pellets can expand dimensionally
during storage by relaxation and/or moisture absorption.
Therefore, the relaxed density of a single pellet needs to
be determined after about two weeks of pellet production.
Tapped density, also known as apparent powder density, is
measured by filling a known volume contained with pulver-
ized biomass or pellets and tapping at least five times to
attain optimal packing. The tapping density can be deter-
mined by dividing the mass of biomass or pellet by the con-
tainer volume.
Moisture resistance
Water resistance is a vital parameter for biomass pellets as
it affects the storage and transportation behavior. Moisture
is necessary during biomass densification as it provides a
binding effect. Moisture adsorption should be stringently
controlled during storage and transportation because adsorp-
tion of moisture encourages microbial activity leading to the
degradation of pellets. This decreases the strength of pellets
and weakens the interparticle bonding, thus reducing the
density and resulting in high transportation cost and low
energy content.
The common methods of determining moisture resist-
ance of pellets are immersion test and moisture adsorption
test under controlled environments. In the case of moisture
adsorption measurements, pre-dried pellets are placed in a
humidity chamber at 30 °C and relative humidity of 90%
(Azargohar et al. 2019a). The weight difference between the
dry weight at the beginning and the equilibrated weight after
moisture absorption after 48 h can be used to calculate the
moisture uptake rate. In the case of the immersion test, pel-
lets are immersed in water for 24 h and the weight difference
indicates the moisture adsorption (Bai et al. 2018).
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 Environmental Chemistry Letters

Table 3  Characterization techniques for assessing physicochemical, mechanical and fuel properties of biomass pellets
Category Significance Properties Methods or techniques Reference

Physical Density significantly affects Unit density Using mass and dimensional Sarker et al. (2021a, b)
costs relating to storage and Relaxed density analyses Sarker et al. (2021a, b)
transportation
Bulk density Displacement method Lestari et al. (2015)
Tapped density Displacement method Webb (2001)
Particle or true density Pycnometer method Webb (2001)
Ability to resist adsorption of Hydrophobicity or moisture Moisture adsorption test Azargohar et al. (2019b)
moisture in humid condi- resistance using equilibrium moisture
tions content and/or immersion
test
The distribution of particles Particle size distribution Sieving methods and particle Hu et al. (2015)
affects flowability, heat dif- size analysis
fusion, reaction rate during
combustion and inter-
particular bonding
Determination of ash com- Inorganic components Inductively coupled plasma Sarker et al. (2020)
position
Chemical Determination of moisture, Elemental analysis American Society for Test- Si et al. (2016)
ash, volatile matter and ing and Materials standard
fixed carbon content
Determination of carbon, Ultimate analysis Carbon–hydrogen–nitrogen– Zhu et al. (2018)
hydrogen, nitrogen, sulfur sulfur–oxygen analyzer
and oxygen
Cellulose, hemicellulose and Biochemical composition National Renewable Energy Stelte et al. (2011b)
lignin Laboratory method
Surface functional groups Chemical composition Fourier-transform infrared Abedi and Dalai (2017)
spectroscopy
Carbon and hydrogen-con- Chemical composition Solid-state nuclear magnetic Azargohar et al. (2019a)
taining compounds resonance spectroscopy
Mechanical Degree of breakage of fuel Durability Tumbling test Gilvari et al. (2019)
pellet
Resistance to stretching and Tensile strength Instron testing machine Gilvari et al. (2019)
pulling
Resistance to squeezing force Comprehensive strength Universal testing machine Gilvari et al. (2019)
Resistance to impact forces Impact resistance Drop test Gilvari et al. (2019)
Binding mechanism Visual observations at micro- Surface morphology Scanning electron micros- Azargohar et al. (2019a)
level copy
Inter-particular bonding and Cross-sectional tomography Computed tomography scan Azargohar et al. (2019a);
void spaces Sarker et al. (2022b)
Porosity and void spaces Pore size distribution Brunauer–Emmett–Teller Sarker et al. (2020)
surface area analysis
Combustion and Calorific value Higher heating value Oxygen bomb calorimeter Shuma and Madyira (2019)
thermal behavior Devolatilization Thermal stability Thermogravimetric analysis Sarker et al. (2022b)
Weight loss with temperature Ignition temperature and Thermogravimetric analysis Odusote and Muraina (2017)
time
Ash or char formation Burnout temperature Thermogravimetric analysis Odusote and Muraina (2017)
Amount of time to com- Combustion rate Odusote and Muraina (2017)
pletely burn a known mass
of fuel
Emission analysis Composition of flue gas dur- Gas chromatography Hrdlička et al. (2016)
ing combustion
Determination of pollutants Emission of particulate Inductively coupled plasma Sippula et al. (2017)
matter and X-ray diffraction
analysis of ash and char

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Environmental Chemistry Letters
Mechanical stability
The mechanical stability of pellets is essential for their
bulk transportation and feeding into reactors, ovens, fur-
naces, pyrolyzers, combustors and gasifiers  (Lu et  al.
2008). There are different methods for evaluating the
mechanical stability of pellets such as compression test
or compressive resistance, drop test or impact resistance
and durability test. The maximum crushing load a pel-
let can withstand before cracking or breaking is known
as mechanical strength. Tensile strength or compressive
strength is the parameter for determining the mechanical
strength of the pellets. Impact resistance shattering is also
referred to as drop resistance. This test could stimulate the
stress experienced while dumping densified items from
trucks onto the chutes into bins or the ground. In this test,
pellets are dropped onto a metal plate from a height of
1.85 m at least four times (Gilvari et al. 2019). The weight
retained stated as the percentage of the initial weight is
known as drop resistance.
Durability is the most common term used for the deter-
mination of pellet stability. The durability of pellets is deter-
mined by the tumbling test. A representative sample of pel-
lets (usually 500 g) is tumbled for 10 min at the speed of 50
rpm in a tumbling can followed by sieving the pellets using
a sieve screen of 3.15 mm and weighing (Gilvari et al. 2019).
The ratio of the mass of fine particles remaining in the sieve
and the initial mass of pellets is known as durability.
Composition
The basic physicochemical properties of pellets include
proximate and ultimate analyses, which provide a basic
understanding of biomasses. The proximate analysis
determines moisture, volatile matter, ash and fixed car-
bon of a material, while the ultimate analysis determines
carbon, hydrogen, nitrogen, sulfur and oxygen content.
The energy content of the pellets can be determined by
an oxygen bomb calorimeter or computed by the modified
Dulong formula using the ultimate composition (Nzihou
et al. 2014; Bai et al. 2018). Biopolymeric composition
of lignocellulosic biomass is also important to measure
the contents of cellulose, hemicellulose and lignin (Akalın
et al. 2017). These contents are usually determined by the
standard National Renewable Energy Laboratory method
(Sluiter et al. 2010). This process involves the removal of
polar and non-polar components such as extractives using
water, ethanol and hexane, followed by two-stage dilute
acid hydrolysis to remove cellulose and hemicellulose
monomers. The percentages of cellulose and hemicellu-
lose were calculated by detecting different sugars in high-
pressure liquid chromatography.
Particle bonding
The binding mechanism of the pellets is crucial since it can
offer pictorial evidence for determining the binding mech-
anism. There are a few techniques to visualize the pellet
structure such as scanning electron microscopy, transmission
electron microscopy, fluorescence microscopy and computed
tomography scanning analysis. Porosity is another parameter
to estimate the strength of pellets. The pellets with higher
pore space offer weaker pellets. Scanning electron micros-
copy, transmission electron microscopy and fluorescence
microscopy techniques usually provide two-dimensional
images of pellet surfaces, which are used to investigate the
morphology and binding pattern of biomass particles within
the pellets. Scanning electron microscopy also determines
the particle bonding in biomass pellets (Azargohar et al.
2019a, b). Castellano et al. (2015) observed small holes and
void spaces among the particles, implying better particle
agglomeration.
The porosity of the pellet can be determined by a com-
puted tomography scan. A computed tomography scan is
typically applied in medical imaging and radiology to elu-
cidate internal images of a body part. However, computed
tomography scans are now made their way to analyze
non-conventional samples such as plant materials, car-
bonaceous products and engineered biomaterials. Micro-
computed tomography has advantages over conventional
scanning electron microscopy and transmission electron
microscopy imaging tools, which are not suitable to visu-
alize the internal arrangement of the whole pellet and the
development of buried cracks from the pellet surface. A
computed tomography scan is a three-dimensional imaging
technology that collects a succession of two-dimensional
X-ray projection images, while the sample rotates through
a 180° angle range. The raw data is converted into a three-
dimensional internal image of the sample using a recon-
struction algorithm. The raw data is then transformed into
a three-dimensional internal image of the pellet sample.
Synchrotron-based computed tomography scan has shown
to offer high sensitivity and phase-based contrast than tra-
ditional X-ray based imaging techniques, thus making it an
excellent tool for visualizing the interior void structure of
pellets, biochar and organic materials (Abedi et al. 2018;
Azargohar et al. 2019a).
Strandberg et al. (2018) used synchrotron-based three-
dimensional X-ray micro-tomography for examining vari-
ous charred pellets produced from poplar and wheat straw.
They studied how internal cavities, cracks and ash layers
evolved during the conversion process. They discovered
that poplar ash produced a thin ash coating on the surface
of char during carbonization. Potassium and calcium sili-
cates with high viscosity were also detected on the surface
of wheat straw char in the form of bubble-like structures.
13

Advanced characterization techniques could aid in the
development of more precise and adaptable fuel particle
conversion models as well as offer an understanding of the
ash production process in biomass densification research.
Micro-computed tomography scan has also been deployed
by other researchers to study the structural integrity of
pellets and bio-based materials (Rudolfsson et al. 2017;
Azargohar et al. 2019b; Sarker et al. 2022b).
Sarker et al. (2022b) used a Synchrotron-based micro-
computed tomography scanning technique to investigate
the internal constructions of biomass fuel pellets and to
determine their porosity. Lower porosity referred to low
void space and potential high mechanical strength and den-
sity of pellet. As discussed earlier, pellets with low bulk
density can add to the logistic costs relating to their stor-
age and transportation, while low mechanical strength can
increase the release of biomass dust and fines during han-
dling and shipping operations of pellets. Thus, it is decisive
Fig. 8  Synchrotron-based micro-computed tomography images of
biomass fuel pellets. Reproduced with permission from Sarker et al.
(2022b). Note: P1 (raw canola residue), P2 (torrefied canola residue),
P3 (torrefied canola residue with 10% lignin), P5 (torrefied canola
13
Environmental Chemistry Letters
to know the inside cavities and pore space of fuel pellets.
Fig. 8 illustrates the micro-computed tomography of pellet
produced from torrefied canola residue with the addition
of different bio-based additives. Raw canola residue pellet
showed the highest porosity around 15%, while in the case
of torrefied biomass pellet it reduced to 11%. Moreover, the
addition of additives further reduced the pellet porosity to
a certain extent. Pellets made from torrefied canola residue
with lignin, mustard meal, and bio-oil were found to be the
most compact, have the lowest porosity, and have the fewest
interconnected pores.
The surface functional groups of pellets may alter at the
time of densification, which is measured using Fourier-trans-
form infrared spectroscopy. Si et al. (2016) found that adding
a carboxymethyl cellulose binder to the biomass densifica-
tion process increased carbon–hydrogen bonding because it
sequestered oils and waxes onto the pellet surface. Thermo-
gravimetric analysis can determine the thermal stability and
residue with 10% mustard meal), P6 (torrefied canola residue with
15% pyrolysis oil) and P14 (torrefied canola residue with 10% lignin,
10% mustard meal and 15% pyrolysis oil)
Environmental Chemistry Letters
ignition and burnout temperatures of biomass pellets. Using
X-ray diffraction and nuclear magnetic resonance spectros-
copy, Azargohar et al. (2019a) discovered that pelletization
did not affect the cellulose structure of canola hull pellets.
Raman spectroscopy is also used to evaluate the fingerprints
of the main components of the biomass precursor and pel-
lets as it is more sensitive than Fourier-transform infrared
spectroscopy (Abedi and Dalai 2017).
Energy applications of biomass pellets
There are numerous applications of fuel pellets ranging from
household cooking and residential heating to power plants
at an industrial scale as exemplified in Fig. 9.
Residential heating and cooking
Fuel pellets are commonly used in household boilers and
stoves. In most European countries, the major fuel source for
household stoves is wood pellets. Recently, many researchers
have focused their interest on the suitability of agricultural
biomass pellets for use in domestic stoves. However, this
requires determining the effect of pellet quality and operat-
ing conditions on emissions of gases, particulate matter and
ash. It has been reported that the quality of fuel pellet signifi-
cantly affects the emissions of both gaseous and particulate
matter (Garcia-Maraver et al. 2014). Particle density and the
length-to-diameter ratio of fuel pellets have a great influence
on the CO emissions of biomass pellets.
Wohler et al. (2017) examined the impact of the length
of pellet on the performance of solid fuel stoves using three
softwood pellet samples of varying lengths. The results
Fig. 9  Main  energy-based applications of biomass fuel pellets. Bio-
mass pellets can be applied in co-firing, pyrolysis, gasification, com-
bustion, burning, cooking and heating
revealed that the emission of CO decreased from 185 to 27
mg/m3, respectively when using a long pellet instead of a
short pellet in a nominal operational load of a stove. Mean-
while, the emission of particulate matter also reduced dra-
matically from 882 to 37 mg/m3. However, the length and
shape of pellets also influence the emissions as long pellets
emit more gaseous and particulate matter.
Cardozo et al. (2014) compared fuel pellets with 6 mm
diameter produced from sunflower husk, bagasse and Bra-
zil nut against wood pellets of the identical size in a pellet
burner and observed a higher oxygen content in the flue gas,
quicker ash removal cycles and reduction in fuel power input
when non-woody pellets were used. They also reported that
the proportional conversion of elemental nitrogen to NO and
elemental sulfur to S­ O2 was greater for wood-based pellets
compared to those for other biomass pellets.
Verma et al. (2011) compared the combustion behavior
of fuel pellets produced from sunflower husks to those from
other biomasses such as apple powder, wood, straw and
peat in a domestic pellet boiler. They noticed that the CO
emission was maximum for peat-based pellets, especially
13 times higher than wood-based pellets. The criteria for
assessing the quality of biomass fuel pellets have been set
to enhance the efficiency of combustion and eliminate tech-
nical issues in energy conversion equipment. To promote
the growth of fuel-flexible combustion units, it is critical to
assess the suitability of other biomass-based pellets instead
of the traditional wood-based pellets.
Combined heat and power generation
The worldwide industrial clean energy generation relies
heavily on wood-based biomass pellets. This is in contrast
to the fossil-based power generation that uses gasoline and
coal to generate electricity, while at the same time, releas-
ing massive amounts of greenhouse gas emissions and pol-
lutants. To reduce industrial emissions, the usage of bio-
mass pellets can be a sustainable and long-term option for
combustion or co-firing combined heat and power systems.
Therefore, high-quality coal-like fuel pellets are required to
retrofit the fuel input of industrial power plants with renew-
able sources rather than fossil fuels. However, usage of non-
woody biomass pellets in industrial applications is restricted
due to high ash content as it leads to sintering and clinker
formations.
High hydrophilicity also causes problems in handling and
transportation with water adsorption in moist environments.
To make biomass more appropriate for industrial applica-
tions, torrefaction can be applied as a thermal pretreatment
as discussed earlier. Proskurina et al. (2017) assessed the
potential of torrefied biomass in diverse industries includ-
ing power and non-power sectors. They recommended that
torrefied products can efficiently replace fossil fuel at an
13

industrial scale. Besides combustion and co-firing, biomass
pellets can also be used in other industries such as paper and
pulp, ceramic, glass making, metallurgy and cement making
leading to reduced greenhouse gas and particulate emissions.
Wang et al. (2015) investigated the incorporation of bio-
mass such as char, wood pellets and torrefied material to
replace pulverized coal in blast furnaces of steel industries.
Their study reported that wood pellets can reduce the overall
emission by 6% while 28% for charcoal alone. Suopajarvi
et al. (2017) recommended the usage of biomass-based fuels
in iron and steel-making industries from the viewpoints of
technical potentials and restraints, environmental risks and
economic feasibility. Their study suggested that biomass-
based reducing agents have a great potential to be used in
various ratios with coal in iron and steel-making processes.
Another study reported that the total C ­ O2 emissions can
be reduced by 11% if the utilization of charcoal as a fuel
increase from 23 to 33% in Brazilian steel and iron indus-
tries (Pinto et al. 2018). The use of pellets produced from
sewage sludge could be a potential approach for improving
the immobilization of heavy metals apart from their fuel
applications (Xiao et al. 2015b). The boiler efficiencies of
fuel pellets obtained from co-pelletization of sawdust and
municipal solid waste ranged up to 77% (Xiao et al. 2015a).
This was higher than that generated from sludge and wood-
chip co-combustion. Recently, pulp and paper industries
globally have expressed interest in the use of biomass fuel
pellets to broaden the industry’s scope outside its main busi-
ness (Proskurina et al. 2017). Although there is a scarcity
of information on the use of fuel pellets in industrial sectors
at the moment despite the mounting interest in the utility of
biomass fuel pellets.
Gasification for gaseous fuel production
Another promising application of biomass fuel pellets is
recognized in gasification to generate bio-syngas, a gaseous
fuel comprising predominantly of CO and ­H2 along with
trace levels of ­CH4. Syngas can be further utilized as a gase-
ous fuel for Combined heat and power sectors or to produce
value-added chemicals by gas-to-liquid processes such as
Fischer–Tropsch synthesis. Densification and torrefaction of
biomass significantly improve the gasification performance
and gas quality. Gas yields, lower heating value of gases
and carbon conversion efficiency are significantly improved
during the gasification of densified biomass compared to
raw feedstocks (Sarkar et al. 2014). However, the quality
and composition of gaseous products and gasification per-
formance greatly depend on the quality as well as physical
properties of fuel pellets (Pradhan et al. 2018b).
Prasad et al. (2015) stated that the energy content of pro-
ducer gas increased by gasifying pellets with smaller diam-
eters such as 12 mm versus 17 mm. It was because a higher
13
Environmental Chemistry Letters
surface area of pellets provided better combustion perfor-
mance. The smaller the particle size of the biomass particle
in the pellets, the denser the biomass pellet becomes. This
plays a vital role in reducing the applied pressure during
biomass compaction. Besides pellets produced from biomass
with smaller particle sizes, higher gasification temperature
led to higher gas yields, better process efficiency, low tar
yield and greater energy content of gases.
The bulk density of fuel pellets also influences the gas
composition. A study demonstrated biomass pellets with
high bulk density produced gas with a high concentration
of ­H2 and ­CO2, while CO concentration was low (Schweitzer
et al. 2018). The authors also mentioned that low bulk den-
sity materials cause lower fuel conversion leading to reduced
gas yields. According to Kallis et al. (2012), the ash content
and durability of pellets have a substantial impact on the
produced gas quality and quantity.
Techno‑economy of biomass densification
Since the wood pellet market has been steadily growing both
in industrial and residential sectors, there is a great potential
for using different waste biomass to produce fuel pellets.
However, the economic analysis is important to evaluate
the viability of the densification and conversion processes
including logistic and operational costs of pelletization, stor-
age, transportation and conversion as well as environmental
benefits and risks relating to emissions of greenhouse gases,
particulate matter and byproducts.
Pradhan et al. (2018a) studied the economic feasibility
of fuel pellets produced from agricultural wastes using a
pelletizer with a capacity of 2 tons/day. They concluded
that pelletization can be profitable when the pellet price is
higher than $120/ton. However, the cost of raw materials
was the most influential factor in cost analysis. Mupondwa
et al. (2012) reported that a positive net present value can be
obtained for pellets produced from wheat straw at a process-
ing capacity of 12 ton/h if the price is higher than $100/ton.
They also mentioned that a pellet plant with a low capac-
ity of 2–6 ton/h could require a high price of more than
$140/ton to reach a positive net present value compared to
that of a high-capacity facility, especially 18–35 ton/h. A
study reported that the lowest selling price of torrefied pel-
lets could be $207/ton depending on the cost of feedstocks
and product yield from torrefaction (Manouchehrinejad
et al. 2021). In addition, the growth in plant capacity up to
200,000 tons/year can reduce the selling price by up to 10%.
Shahrukh et al. (2016) mentioned that the cost of a wood-
based pellet and steam-treated pellets can be in the range
of $95–105/ton and $146–156/ton, respectively. Song et al.
(2017) reported that a pellet plant with a capacity of 50,000
tons/year based on corn straw biomass from five neighboring
Environmental Chemistry Letters
villages could be economically feasible compared to a plant
with a capacity of 10,000 tons/year. They have suggested
that the smaller plant can be economically profitable at a
higher pellet price excluding tax subsidies or the promotion
of carbon credits.
Agar (2017) compared the costs of producing torrefied
pellets with raw pellets. Conventional raw pellets had a
higher annual production cost (€7.05 M) than torrefied pel-
lets (€6.11 M). Furthermore, torrefied pellets had a higher
specific cost of €95.54/ton than raw pellets. Chai and Saf-
fron (2016) compared the production cost of pellets in three
different scenarios such as raw pellets, lightly torrefied pel-
lets and severely torrefied pellets. They reported the pro-
duction cost of lightly torrefied pellets compared to other
scenarios. Biomass field conditions and climate conditions
are also significant parameters contributing to the quality
and production cost of pellets. Torrefied pellets have a higher
production cost than raw pellets because of the cost of pre-
treatment (Pradhan et al. 2019). However, additional costs
can be offset by long-distance transportation and logistics.
Energy-dense and hydrophobic solid fuels such as torrefied
pellets have a wide range of industrial applications as dis-
cussed earlier.
Conclusion
Exploring the potential of lignocellulosic biomass to pro-
duce solid, liquid and gaseous fuels is extremely necessary
to counteract the rising energy demands and pollution prob-
lems. This article conducted a thorough literature review
of recent research on biomass densification, pelletization
parameters, pellet formulations and end-uses. The com-
position of biomass such as moisture and particle size as
well as contents of cellulose, hemicellulose and lignin have
significant impacts on the physicochemical and mechanical
features of biomass pellets. Moreover, pretreatment carried
out on biomass feedstocks may also affect the pelletization
process remarkably. This paper critically examines various
pre-processing techniques for improving pelletization and
pellet quality. The quality of fuel pellets is critical for stor-
age, handling, shipping and international trade. Pellets can
be used in a variety of energy and power sectors such as resi-
dential stoves, combustors, gasifiers and industrial boilers. It
has been suggested that there is a huge market for biomass
pellets as a substitute for its fossil fuel counterparts such
as coal in the energy and power sectors. Hence, advanced
research is recommended on optimizing and standardizing
pellet quality, design of conversion systems, integrated con-
version routes, co-processing of feedstocks and recycling
of process byproducts to establish a circular economy, cost
efficiency and environmental sustainability.
Funding  The authors acknowledge the funding received from BioFu-
elNet Canada; Agriculture and Agri-Food Canada (AAFC); Agricul-
tural Development Fund (ADF) by the Government of Saskatchewan,
Canada; the Natural Sciences and Engineering Research Council of
Canada (NSERC); and the Canada Research Chairs (CRC) Program.
The University of Saskatchewan Dean’s Scholarship awarded to Dr.
Tumpa R. Sarker is also acknowledged.
Declarations 
Conflict of interest  The authors declare that they have no conflict of
interest.
Consent for publication  All authors agree to publish this article in
Environmental Chemistry Letters.
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