Carbon Capture Science & Technology 1 (2021) 100005

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Carbon Capture Science & Technology

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Better use of bioenergy: A critical review of co-pelletizing for biofuel

manufacturing
Xuyang Cui 1,2,∗, Junhong Yang 1,2,∗, Zeyu Wang 1,2, Xinyu Shi 1,2
1
Key Laboratory of Efficient Utilization of Low and Medium Grade Energy, MOE, Tianjin University, Tianjin 300350, China
2
School of Mechanical Engineering, Tianjin University, Tianjin 300350, China

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

Keywords: Better and more efficient use of biomass energy is seen as a favourable option for reducing carbon emissions.
Bioenergy Biomass pellet fuel is one of the most common and important ways of utilising biomass energy. The use of diverse
Solid fuels biomass resources with different properties for pelletizing is a current research hotspot. This paper provides an
Pellets
innovative overview of co-pelletization technology for biomass pellet fuels. The chemical composition of various
Co-pelletizing
types of biomass is classified and the influence of different biomass matrix feedstocks and pelletizing operating
Fuel quality
Process parameters parameters on pellet quality and pelletizing process is summarized. The research results indicate that the natural
chemical fraction of biomass has a significant influence on the pelletizing process and fuel quality. Furthermore,
co-pelletizing can be divided into biomass-biomass co-pelletizing and biomass-non-biomass co-pelletizing. Com-
mon co-pelleting combinations include: woody and herbaceous crop co-pelleting; woody or herbaceous crops
with high starch and oil content (e.g. microalgae, peanut shells, etc.); mixed pelleting of different parts of the
same crop (e.g. bark and leaves of the same quality); co-pelleting of biomass with solid waste (e.g. municipal
sludge, waste paper, etc.). Crop types such as oil and sugar used for co-pelletizing with herbaceous and woody
crops help to reduce energy consumption in the preparation of biomass pellet fuel and improve the quality of the
pellets. Co-pelletization of non-biomass-based materials (domestic production waste, inorganic additives) with
biomass also facilitates the pelletizing process and improves the quality of pellet fuel. It is obvious that mixing
different raw materials for co-pelletizing is considered a promising way for upgrading biomass pellet and that eco-
nomical, environmentally friendly and sustainable raw materials are prerequisites for co-pelletizing. Moreover,
co-pelletizing seems to be a strong option for enhancing the competitiveness of biomass pellet fuel production at
scale in the future.

1. Introduction of total global energy consumption, of which 67.2% was contributed by

With the increase in the global demand for energy, the excessive
use of fossil fuels has led to many environmental problems due to ex-
cessive CO2 emissions (Hu et al., 2018). In order to cope with the
challenges posed by excessive CO2 emissions, making full use of re-
newable energy has become an important initiative to reduce carbon
emissions (S., 2021). Especially after the Paris Agreement in 2015, re-
newable energy has been given the expectation to limit climate change
to less than 2°C of temperature rise compared to pre-industrial levels
(Xiaotong et al., 2021). The Chinese government has also recently de-
clared that it will achieve "carbon peaking by 2030 and carbon neutral-
ity by 2060" (Sheng et al., 2021). Renewable energy will play an impor-
tant role in the world’s future energy mix as it is clean and sustainable.
According to WBA (2020) data, in 2018, the total primary energy supply
from renewable sources was 82.7 EJ, accounting for approximately 18%
biomass (WBA, 2020) (as shown in Figure 1) (WBA global bioenergy
statistics 2018). Total energy from biomass sources (TPES) such as mu-
nicipal waste, industrial waste, solid biomass, liquid biofuels and bio-
gas was 55.6 EJ, an increase of 1.2% over the previous year. In 2018,
Asia had the highest TPES from renewable energy sources, followed by
the Americas and Africa with 40%. Bioenergy accounts for a significant
share across all continents, ranging from 36% in Oceania to 95% in
Africa.
In addition, among renewable energy sources, biomass has a broad
potential for application as a carbon-neutral energy source, as it does
not add a net amount of carbon dioxide to the atmosphere (in Figure 2)
(Ahmed et al., 2021). The use of agricultural residues and organic waste
as fuel substitutes will reduce emissions from open burning and landfills
respectively, and thus be a source of income for all stakeholders. In this
context, biomass has a great potential as a renewable and sustainable
source for bioenergy production. Especially in China, the construction

∗
Corresponding authors.
E-mail addresses: cui_xuyang@tju.edu.cn (X. Cui), yangjunhong@tju.edu.cn (J. Yang).

https://doi.org/10.1016/j.ccst.2021.100005
Received 6 September 2021; Received in revised form 8 October 2021; Accepted 8 October 2021
2772-6568/© 2021 The Author(s). Published by Elsevier Ltd on behalf of Institution of Chemical Engineers (IChemE). This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/)
X. Cui, J. Yang, Z. Wang et al. Carbon Capture Science & Technology 1 (2021) 100005

Figure 1. Biomass energy and contribution to world energy (∗ Data from WBA 2020)

Figure 2. Carbon cycle throughout biomass production and utilization

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X. Cui, J. Yang, Z. Wang et al.
Figure 3. Global biomass fuel supply and share of biomass solid fuels in biofuel (Data from WBA2020) (World Bioenergy Association 2020)
of a "beautiful countryside" has become one of the most important ele-
ments of social development in recent years, and with the introduction
of various biomass incentives, it is imperative to actively promote the
use of biomass energy in China (Chen et al., 2016).
Biofuels are liquid, gaseous and solid fuels produced primarily from
biomass, such as ethanol, methanol, biodiesel, Fischer-Tropsch, hydro-
gen, methane, etc (Gebregiorgis et al., 2021). Biomass is supplied from
a variety of feedstocks - wood fuel, forestry residues, charcoal, pellets,
agricultural crops and residues, municipal and industrial waste, biogas,
biofuels, etc (Alizadeh et al., 2020). As shown in Figure 3, WAB2020
data shows a global biomass supply of 55.6 EJ, of which 85% comes
from solid biomass, including wood chips, wood pellets and traditional
biomass resources. Liquid biofuel accounts for 7% and municipal and in-
dustrial waste accounts for 5%, followed by biogas at 3% (WBA global
bioenergy statistics 2018). Solid biomass products such as wood chips,
pellets and charcoal, mainly from the forestry sector, account for the
majority of the global biomass supply.
Biomass demonstrates two main disadvantages as a fuel source,
namely low bulk density (or energy density) and high costs in han-
dling, transport and storage (He et al., 2018). To address these issues,
biomass solid fuels have been developed. Common biomass feedstocks
used to make solid fuels are wood industry waste, agricultural and forest
residues, energy crops, etc. Biomass solid fuels produce less particulate
emissions and possess a higher energy density than their raw form and
other conventional biomass fuels (He et al., 2018, Tomáš et al., 2021,
I.S. et al., 2021). In addition, the regular geometry and standard dimen-
sions allow for compact storage, easy handling, and regular feeding in
large-scale applications (I.S. et al., 2021). Among all kinds of solid fuels,
woody solid fuels are the biomass commonly used in modern bioenergy
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Carbon Capture Science & Technology 1 (2021) 100005
(Stelte et al., 2012). Among the various types of biomass solid fuels,
pellets and briquettes are the most common forms in solid biofuel pro-
duction (Pradhan et al., 2018). Depending on the application, relevant
standards specify that the diameter of pellet fuels should be less than or
equal to 25 mm, while that of rod (block) fuels should be greater than
25 mm (Zhang, 2012). In general, pelletizing rods with larger diameters
can be selected due to favourable compression properties, such as rice
stalks, rhododendron walls and manzanita. However, the larger the di-
ameter, the lower the density after pelletizing (≤1 g/cm3 ) due to the re-
duced pressure per unit area (Stelte et al., 2012). Additionally, there is a
difference in the production technique and market demand between pel-
lets and briquettes (Pradhan et al., 2018).Both biomass briquettes and
biomass pellets are densely formed from biomass raw materials under a
certain pressure and temperature, and the main difference between the
two processes is the difference in the die size of the two manufacturing
equipment (Pradhan et al., 2018). i) Briquettes. They are 75 to 300 mm
in diameter and length, respectively, and are generally in cylindrical
form. They are larger in size than pellets and are suitable for medium
and large industrial heat plants (Dinesha et al., 2019). ii) Pellets. They
are cylindrical in diameter and length from 50 to 90 mm, and the most
commonly used are pellets with 6 and 8 mm in diameter and up to 40
mm in length. They are extensively used in small devices such as residen-
tial cookers, gasifiers, etc. This paper takes pellet as the main research
object in view of its wide application (Pradhan et al., 2018).
Biomass is abundant and diverse. For example, in China, the market
price of pellet fuel made from wood chips, bark and crop straw is RMB
700 (±100) per tonne, RMB 550 per tonne and RMB 400 per tonne,
respectively (Wang et al., 2013). The selection of raw materials in the
biomass pellet fuel industry is crucial as there is a great difference in the
X. Cui, J. Yang, Z. Wang et al.
type of raw material, preparation process and fuel quality, which affects
the market price (Pradhan et al., 2018). Furthermore, a lot of processes
are involved in preparing biomass pellet fuel, including crushing, siev-
ing, drying, mixing and pelletizing, of which pelletizing process alone
contributes approximately 50 % of energy consumption (Mostafa et al.,
2019). In recent years, many studies have focused on different types of
biomass for pelletizing, such as garden waste (Pradhan et al., 2018), soy-
bean (Scatolino et al., 2018), sugarcane bagasse (Scatolino et al., 2018),
cherry kernels (Dołżyńska et al., 2019), fallen leaves (González et al.,
2020), chamomile waste (Zawiślak et al., 2020), sunflower seed hulls
(Cui et al., 2019), peanut shells (Jiang et al., 2020), walnut hulls
(Lisowski et al., 2019), and walnut shells (Lisowski et al., 2019), corn
cobs (Kaliyan and Morey, 2010), microalgae (Miranda et al., 2018)
and other emerging biomass solid wastes. In addition, co-pelletizing
by mixing different materials and optimizing pelletizing parameters
seem to be feasible routes to obtain high quality pellets. For exam-
ple, Zvicevičius et al (Zvicevičius et al., 2018) studied the improve-
ment of water content in the pelletization of a herb with a cuckoo wall;
Cui et al (Cui et al., 2019) conducted a multi-parameter optimisation
study of parameters such as water content, pelletizing temperature and
pelletizing pressure when using sunflower seed hulls for pelletization
to obtain higher quality sunflower seed hull pellets; Rahaman et al
(Rahaman and Salam, 2017) studied the synergistic effect of adding
wood chips to rice straw pellet and reducing pressure to improve the
density of pellet fuel. At present, in order to make biomass pellet fuels
better suited to the market and to make better use of biomass resources,
the biomass pelletizing of different matrix materials has been indepen-
dently and extensively studied by numerous scholars. However, there is
little systematic research on the co-pelletizing of different biomass mix-
tures and their process parameters. Therefore, it is necessary to provide
a systematic review of co-pelletization technology for biomass pellet
fuels.
In this paper, recent research on co-pelletizing of different biomass
feedstocks is systematically reviewed, the chemical composition of
various types of biomass is classified and the selection of various
pelletizing process parameters and pelletizing methods for different
biomass substrate feedstocks is summarized. This study provides guid-
ance for optimising pellet production process and improving pellet
quality.
2. The impact of the composition of feedstock on biopellet
As can be seen from Figure 4, a great deal of effort has been invested
in the development of biomass energy in recent years. Diverse potential
biomass feedstocks from different sources can be used to produce biofu-
els, including woody biomass, herbaceous biomass, aquatic biomass, an-
imal waste, etc (Saeed et al., 2021). At the same time, the main concerns
for bioenergy production are to reduce production costs, improve energy
use efficiency, reduce greenhouse gas emissions, and improve the com-
patibility of fuel utilisation systems. Biofuels are broadly divided into
primary and secondary biofuels. Primary biofuels are used in their un-
processed form, mainly for heating, cooking or electricity generation,
and include fuelwood, wood chips and pellets. Secondary biofuels in-
cluding ethanol, biodiesel etc are produced by processing biomass and
can be used in automotive and industrial processes. Secondary biofuels
are subdivided into first-, second- and third-generation biofuels based
on raw material and production technology (Liu et al., 2020).
There are various biomasses used in biomass pellet fuels, among
which forest wood chips and waste straw are more commonly used raw
materials. In terms of chemical composition, these biomasses mainly
contain lignin, cellulose, hemicellulose, protein, lipids, water, ash and
other components (García et al., 2018, Demirbaş, 1999, F.O., 2008),
and the relationship between these chemical components is shown in
Figure 5. It can be seen from the figure that lignin, cellulose and hemi-
cellulose are the main components that make up the cell wall of plants
and are also the main components contained in plants, which constitute
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Carbon Capture Science & Technology 1 (2021) 100005
the basic morphology of plants. Structurally, lignin is bound to cellulose
and hemicellulose through covalent and non-covalent bonds, forming
a complex three-dimensional inhomogeneous network (U.B. and K.A.,
2016), and their structural relationships are shown in Figure 5.
Although the chemical components that make up a plant are roughly
the same, different types of plants, even the same plant at different
stages of growth and in different regions, contain different levels of
chemical components, and the content of chemical components has
a significant impact on biomass pelleting. The main chemical compo-
nents and contents of several plants are listed from Table 1. The con-
tent of certain chemical components varies considerably from plant to
plant. In general, for woody plants such as spruce, willow fir, horsetail
pine and cypress, lignin and cellulose account for around 30% and 40-
50% respectively, higher than herbaceous plants such as wheat straw,
rice straw and corn stalks (10-20%, <40%), while herbaceous plants
such as wheat straw have a hemicellulose content of 20-25%, higher
than herbaceous plants such as spruce (<20%). The content of lignin in
woody plants also varies with softwoods containing more lignin than
hardwoods (Zhang, 2012). The water content of plants measured in the
table is about 10%, but it is greatly affected by growth stage and stor-
age time (Zhang, 2012). The ash content of different plants varies con-
siderably: woody plants contain very little ash, usually no more than
1%, while herbaceous plants contain large amounts of ash. In general,
a small amount of protein (<1%) is found in agroforestry biomass, but
some organisms such as legumes and microalgae contain large amounts
of protein, which can be up to 30% or more (Soto-Sierra et al., 2018,
Phusunti et al., 2018, Xu et al., 2019).
The chemical composition of biomass has a significant influence on
the pelletizing process and fuel quality, including pelletizing energy con-
sumption, damage resistance (pelletizing strength, durability) and hy-
drophobicity. The properties of various chemical components and their
influence on pelletizing have been mentioned in many studies, directly
or indirectly. Table 2 summarises the main chemical components of sev-
eral biomasses, as well as their properties, their influence on pelleting
and some typical feedstock types.
In conclusion, different chemical components play different roles in
the process and parameters of biomass pelletizing. Lipids, moisture and
other organic components can all play a lubricating role in pelletizing,
thus reducing pelletizing energy consumption. Lignin, cellulose, hemi-
cellulose, protein and a moderate amount of moisture all play a positive
role in the damage resistance of pellets. Lipids and other organic com-
ponents do not contribute to damage resistance. Lignin can play a facil-
itating role in the hydrophobicity of pellet fuels, while hemicelluloses
tend to absorb water and play an inhibiting role.
3. The impact of operating parameters on biopellet
Pellet fuel is one of the most typical solid fuels. Pelletizing is a key
step in the preparation of biomass pellets, a process that involves many
parameters such as the moisture content of the raw material, the pres-
sure and temperature applied by the pelletizing equipment, as well
as the energy consumption of pelletizing and the size of the pellets.
There are many different ways of pelletizing. Depending on pelletiz-
ing method, there are hot press pelletizing, cold press pelletizing and
charring pelletizing (Qian, 2003, Zhou et al., 2016). All biomass feed-
stocks are obtained by extrusion in a die, and the appropriate solid fuel
is obtained by controlling the pressure, temperature and diameter of
the pelletizing equipment. Figure 6 shows the process of compression
of biomass feedstock into pellet fuels entering different types of pel-
letizing equipment. As can be seen from the diagram, pellets are mainly
obtained by longitudinal compression and deformation of the feedstock
within the die. Typically, biomass feedstocks for pelletizing are mainly
forest wood chips and straw. For different types of biomass feedstocks,
differences in their composition, microstructure, fluidity and moisture
content lead to different process parameters in the pelletizing process
(Zhang, 2012, Kong, 2010). Based on relevant experimental studies of
X. Cui, J. Yang, Z. Wang et al. Carbon Capture Science & Technology 1 (2021) 100005

Figure 4. Mapping of common biomass

Figure 5. Structural relationships of lignin, cellulose and hemicellulose (Zhang, 2012)

Table 1
Main chemical composition of different biomasses (Dołżyńska et al., 2019)

Type Moisture(%) Ash (%) Protein (%) Cellulose (%) Hemicellulose (%) Lignin (%)

spruces 10.97 0.73 0.62 46.92 17.48 28.43

Liu Fir 10.48 0.35 0.80 48.37 17.8 32.47
Masson pine 11.47 0.33 0.86 51.86 15.08 28.42
cedar 10.28 0.41 0.89 44.16 15.62 32.44
wheatgrass 10.65 6.04 - 40.40 25.56 22.34
rice straw 11.53 14.15 - 36.73 21.08 9.49
corn stalks 9.64 4.66 - 37.68 24.58 18.38

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X. Cui, J. Yang, Z. Wang et al. Carbon Capture Science & Technology 1 (2021) 100005

Table 2
Influence of typical biomass chemical composition on pelletization

Chemical Characteristics Effect on pelletizing Raw material types Ref.

composition

Lignin An aromatic compound that
plasticizes and becomes
viscous at a certain
temperature (50-100°C).
Cellulose Insoluble in water, high
toughness.
Hemicellulose Highly absorbent and easily
hydrolyzed to lignin.
Carbohydrate High temperature plasticized
and tacky.
Lipids Easy to degrade at high
temperatures and has
lubricating properties.
Other organic Lubricating, easy to
components decompose at high
(aromatics, waxes, temperature, prone to
terpenes, etc.) greenhouse gases and
carcinogens.
Moisture content A major component of
biological growth and
metabolism.
Ash An inorganic substance
consisting of chlorine and
potassium that is not
combustible.
Heating promotes the bonding between raw Woody plants (about (Zhang, 2012, Pei et al.,
material particles and improves pellet strength. It 30 %), softwoods > 2012, Stelte et al., 2011,
is not easy to absorb water and can improve hardwoods. Whittaker and Shield, 2017,
hydrophobicity of pellet. Heiss-Blanquet et al., 2011)
Beneficial to pellet strength. Woody plants (40 - (Xu et al., 2019,
50 %) Angulo et al., 1995,
Rumpf, 1962, Du, 2011)
Hydrolysis promotes bonding between particles. Herbaceous plants (Pei et al., 2012, Du, 2011,
However, it reduces the hydrophobicity of the fuel. (>20 %) Zhang et al., 2013)
It facilitates the bonding between particles and Microalgae, soy (Soto-Sierra et al., 2018,
improves the strength of pelletizing. Their (>30 %) Phusunti et al., 2018,
structural differences and denaturation also affect Xu et al., 2019, Kaliyan and
the granulation effect. Morey, 2008, B.J. et al.,
1999, Chai, 2013,
Winowiski, 1988,
Wood, 1987)
Reduces friction between the raw material and the Soy, microalgae, etc. (Phusunti et al., 2018,
die during pelletizing, and reduces energy B.J. et al., 1999,
consumption for pelletizing. However, it will Hosseinizand et al., 2018,
reduce the durability of the pellet fuel. Samuelsen et al., 2018,
Kousoulaki et al., 2016)
Lubricates during pelletizing, but durability is Less in general (Whittaker and Shield, 2017,
reduced. The pelletizing content should not be biomass Stelte et al., 2011,
excessive. Florentino-Madiedo et al.,
2018)
Has an adhesive effect. Reduces the plasticization Undried, fresh (Zhang, 2012, Adapa et al.,
temperature of lignin, which in turn reduces the biomass 2011, Nielsen et al., 2009,
pelletizing temperature. Acts as a lubricant during Lehtikangas, 2001)
pelletizing. Excessive moisture content also
reduces pelletizing strength.
There is no effect on the pelletizing process, but it Various straw crops (Zhang, 2012, Wang, 2017)
can affect the combustion process of the pellet
fuel, resulting in coking and slagging in the boiler.

pelletizing, Table 3 lists the relevant process parameters for pelletizing
several different types of biomass feedstock.
The size of the pelletized fuel varies due to differences in pelletiz-
ing equipment. As displayed in Table 3, the type of raw material pel-
letized has an effect. Li et al (Li et al., 2015) selected three organ-
isms representing softwood, hardwood and herbaceous plants, namely
cedar, camphor and straw, respectively, and found that the density of
the pellets was, from largest to smallest, straw, cedar and camphor, with
other things being equal. This suggests that herbs are easier to pellet
than woody plants, and that softwoods are easier to pellet than hard-
woods. Moreover, the easier the pelleting, the higher the density of the
pellets.
The moisture content is an important parameter affecting the pel-
letizing of biomass. The right amount of moisture is conducive to the
bonding between the raw material particles, and can play a lubricat-
ing role. The excessive moisture content will reduce pelletizing effect.
Table 3 shows several types of raw materials with different moisture con-
tents, but moisture content is generally 10-20 %, which is a reasonable
range for most biological materials. Tumuluru et al (Tumuluru, 2014)
found that the optimum moisture content of maize straw was 28-38 %,
and Whittaker et al (Whittaker and Shield, 2017) reviewed the mois-
ture content used for a number of biomass feedstocks, typically 6-13 %
for pine, 8-15 % for straw and 20-25 % for manzanita Since moisture
reduces the plasticisation temperature of lignin and pelleting temper-
ature, the moisture content of lignin-richer biomass feedstocks can be
appropriately increased (Nielsen et al., 2009).
Currently, the most used biomass pelletizing process is hot press-
ing. The pelletizing temperature is an important parameter affecting the
quality of the pellet because heating facilitates lignin plasticisation and
improves the bonding ability between the particles (Jiao et al., 2021,
Riva et al., 2019). For organisms with high lignin plasticisation tem-
peratures, higher temperatures are required to plasticise the lignin and
form solid bridges between the particles, which also indicates that high
pelletizing temperature is required for woody plants with high lignin
plasticisation temperature such as spruce (Stelte et al., 2011). It can also
be seen from Table 3 that the pelletizing temperature of woody plants
such as spruce and sallow quebracho is relatively high, generally above
100°C.
In pelletizing biomass, a certain amount of pressure needs to be ap-
plied to the raw material to facilitate pelletizing. The pelletizing pres-
sure is the maximum compression force exerted by the equipment on
the raw material. Generally, the higher the pelleting pressure, the better
the pelleting results, but the higher the energy consumption required,
which should be kept as low as possible while meeting the criteria. As
herbs are easier to compress, it is less energy intensive to pelletize than
woody plants under the same conditions, whereas there is not much dif-
ference between hardwoods and softwoods (Li et al., 2015), but hard-
woods are not conducive to pelletizing as wood chips are difficult to
pelletize when they are hard and may clog the container (Bradfield and
Levi, 1984, Holm et al., 2006). It is also evident from Table 3 that rice
stalks are much less energy efficient for pelletizing than plants such as
sallow quebracho, spruce and eucalyptus.
The co-pelletization process and physical quality of the pellets may
vary among biomass feedstocks. In practice, in order to improve the
palletizing process and characteristics, the chemical composition and
physical parameters of different feedstocks can be complemented and
coordinated by mixing different types of feedstocks. This co-pelletizing
approach overcomes the shortcomings of poor pellets of some single raw
materials and reduces the wear and tear of equipment (Pradhan et al.,
2018), so it has broad research and application value.

6
X. Cui, J. Yang, Z. Wang et al.
Figure 6. Typical pelletizing equipment and its pelletizing process (Pradhan et al., 2018, Nielsen et al., 2020)
4.1. Co-pelleting between biomass and biomass
Biobased co-pelletizing, characterized by easy access to raw materi-
als and full use of biological resources, has been widely studied. Table 4
lists the research on several types of biomass co-pelletizing. Due to the
energy consumption, strength, durability and water absorption char-
acteristics of pelleting, it is mainly divided into bio-based materials-
high oil plant mixture and herbaceous-woody plant mixture, while other
types of bio-based materials are also added.
Crops such as castor and rapeseed contain large amounts of oil and
grease, and when such plants are added to wood chips, pelleting en-
ergy consumption can be improved because oil reduces friction between
the raw material particles and between the particles and the container.
However, large amounts of oil and grease also reduce parameters such
as pelleting density, strength and durability, and have a negative impact
on pelleting quality (Chai, 2013, Ståhl and Berghel, 2011, Shang et al.,
2014). However, some experiments yielded different results: Cao et al
(Liang et al., 2015) studied the synergistic pelletizing properties of wood
chips and castor cake, and found that the strength of the pelletized par-
ticles was not reduced after the addition of castor cake with high oil
content, because castor cake also contains a large amount of protein
and starch, which have a greater impact on compressive strength, and
these substances can fill the gaps between the raw material particles
in pelletizing, forming solid bridges and hydrogen bonds and thus fa-
cilitating adhesion. Hosseinizand et al (Hosseinizand et al., 2018) and
Cui et al (Cui et al., 2019) studied the synergistic pelleting properties
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Carbon Capture Science & Technology 1 (2021) 100005
of softwoods, hardwoods and chlorella. Their research results indicate
although chlorella improves pelleting quality due to rich protein and
starch despite a large amount of oil and grease. Therefore, when se-
lecting plants with a high oil content for co-pelletizing, plants rich in
protein and starch can also be selected, which will not only reduce the
energy consumption of pelletizing, but also improve pelletizing quality.
According to the current research on co-pelletizing, co-pelletizing can be
broadly classified into two categories: biomass substrate co-pelletizing
and biomass and non-biomass substrate co-pelletizing.
Co-pelletizing of wood chips and straw is a common method for
preparing biomass pellets. Wood chips and straw represent two differ-
ent types of organisms, namely woody and herbaceous, respectively, and
their structures and compositions are quite different. Wood chips con-
tain more lignin and less ash than straw, so they have better strength
and durability and higher ash content when pelletized. The pelleting
quality can be therefore improved by adding wood chips (Rahaman and
Salam, 2017, Serrano et al., 2011, Wamukonya and Jenkins, 1995), but
reduced by adding straw (Lehmann et al., 2012). It can be concluded
that it will be a good option to add an appropriate amount of wood
chips to straw so as to improve the pelleting characteristics of pelleted
pellets.
The characteristics of pelletizing with plant fruits and waste peels
have also been experimentally investigated based on two considerations:
improved pelletizing quality and low cost and easy availability of raw
materials. Organic substances such as lignin, proteins and starch can
improve the pelleting characteristics of biomass feedstocks. Therefore,
X. Cui, J. Yang, Z. Wang et al. Carbon Capture Science & Technology 1 (2021) 100005

Table 3
Pelletizing parameters for common herbaceous and woody biomass

Type Raw Pelletizing Moisture Energy Instructions Ref.

materials density(g/cm3 ) Pressure(MP) Temperature(°C) content(%) consump-
tion(J/g)

herbaceous rice stalks 0.809-1.006 <42 Approx. 120°C About 15 % 7.24-11.35 The effect of particle size on (Wang et al., 2018)
plant pelletizing was explored
stalk of corn 1.136 Approx. 100 12 - The effects of pressure, particle (Mani et al., 2006)
31-137 MP size and moisture on pelletizing
were investigated
Edison Around 1 g/ 156.1-780 cold press 4.3-21.5 - Optimum m[10oisture content (Zvicevičius et al.,
cm3
Cuckoo Wall , up to 9.4 % 2018)
1.07 g/ cm3
Miscanthus 0.391-0.644 - 105 10-30 - Container height-to-diameter (Moon et al., 2014)
sinensis ratio (L/D) between 4.5 and 5,
and optimum water content
20-25 %
reed grass ≥0.65 - Around 80°C Around 15 - Optimum density > 0.65 cm3 , (Larsson et al., 2008)
% durability > 97.5 %
woody plant symbol of 1180-1290 71-176 60-150 2-20 - High temperature, low moisture (Carone et al., 2010)
peace content and small particle size
increase particle durability
sallow - 69-124 70-150 15 Approx. 30 The single pellets of sallow (Chai, 2013)
tannin J/g quebracho and pelleting with
cake meal were studied, where
the optimal temperature was
150°C
spruces 1.0-1.2 ≤300 125-180 10 Average Parametric study of drying (Rudolfsson et al.,
51.8 J/g temperature, moisture and 2015)
granulation temperature
pine 1.08 100 Best at 100°C 4-12 Approx. 28 Under the condition of Particle (Wang et al., 2018)
J/g size 0.15-0.25 mm, moisture
content 4-12 %, temperature
100°C, pressure 100 MP, the
pelletizing effect is the best
Scots pine 1.259-1.276 40.1-61.2 73-103 5.5-5.8 - The smaller the particle size, the (Bergström et al.,
better the particle durability 2008)
-Indicates not measured4 Mixing of different biomass materials and their co-pelletization

Table 4
Research on biomass-biomass co-pelletizing

Type of synergy Raw materials Impact Ref.

Addition of lipid-rich Wood chips + castor Castor cake contains a large amount of oil and grease, and its addition is beneficial (Liang et al., 2015)
biomass cake to reduce the energy consumption of pelletizing and improve the density and
strength of pellets.
Pine wood Canola cake contains a lot of oil and grease, and its addition helps to reduce the (Ståhl and
chips + canola cake energy consumption of pelleting, but the density and durability of pellets will be Berghel, 2011)
reduced.
European Red Rapeseed cake contains a lot of oil and grease, and its addition is beneficial to (Shang et al., 2014)
Pine + Canola Oil reduce the energy consumption of pelleting, but the density and strength of the
pellets are reduced.
Sallow Mixed cake meal can reduce pelletizing energy consumption and water absorption. (Chai, 2013)
extract + cake meal However, due to the high crude protein content of cake meal, the stronger the
adhesion effect, the higher the energy consumption of pelletizing.
Pine wood The large amount of oil in Chlorella reduces the energy consumption of pelletizing, (Hosseinizand et al.,
chips + Chlorella while the protein and starch contained in the pellets improve density, durability and 2018)
water absorption.
Herbaceous + Woody Barley straw + pine The durability of pellets is improved by adding wood chips . (Serrano et al.,
wood chips 2011)
Rice straw + wood The pelletizing pressure is reduced by adding wood chips, but the density of pellets (Rahaman and
chips are increased. Salam, 2017)
Straw + pine wood The durability of pellets is improved by pelletizing a mixture of straw and pine (Wamukonya and
chips wood chips. Jenkins, 1995)
Wood The density and strength of pellets are reduced by adding manzanita to wood chips . (Lehmann et al.,
chips + manzanita 2012)
other Pine wood The natural binding properties of pellets are improved by adding grape pomace with (García et al., 2018)
chips + grape a high lignin content.
pomace
Wood Cassava stems contain a high amount of starch, which increases the durability of (Larsson et al., 2015)
chips + cassava pellets when mixed with wood chips.
stems
Straw + peanut Peanut hulls are cheap and easy to obtain, which improve the quality of pelleting (Bai et al., 2017)
shells when mixed with straw.

8
X. Cui, J. Yang, Z. Wang et al.
the pelleting characteristics of the original biomass substrate, such as
grape pomace rich in lignin (García et al., 2018), and cassava rich in
starch (Larsson et al., 2015) can be improved by adding plants with
a high content of lignin, protein or starch. In addition to choosing a
biobased material that improves the pelletizing properties, the low cost
and easy availability of raw materials is also an important consideration.
Bai et al. (Bai et al., 2017) reduced the cost of fuel preparation and also
improved pelletizing quality by choosing waste peanut shells and straw
for pelletizing.
In addition to the fact that different plants can be pelletized syner-
gistically, even for the same plant, different structures and tissues have
different effects on pelletizing. It has been found that the bark and the
bark-covered trunk are two different parts of the tree, while the chemical
composition of the two is very different: compared to the trunk, the bark
has a higher ash content, about 3-7 times that of the trunk (Chow et al.,
2008, Lerma-Arce et al., 2017); the bark has a higher lignin content
and a lower cellulose and hemicellulose content (Chow et al., 2008). In
addition, structurally, the bark and trunk are different in shape, with
the bark tissue having smaller pores and the trunk tissue having larger
pores, making the trunk easier to compress than the bark (Rezaei and
Sokhansanj, 2018). Choosing the right proportion of bark and trunk for
co-pelletizing is beneficial for optimising the pelletizing characteristics
of the biofeedstock. The synergistic pelletizing effect was better for dif-
ferent straw tissues. Djatkov et al. (Djatkov et al., 2018) found that the
pelletizing characteristics of corn cob were better than that corn straw
through the synergistic pelletizing of corn straw and that the mixture
improved the pelletizing density and strength of the straw. Thus, pel-
letizing can be achieved by synergizing different tissue structures of the
same plant, which not only reduces the selection of other plants, but
also achieves the full utilisation of biological resources, so it is worth
considering in future research on biomass pellet fuels.
4.2. Co-pelleting between biomass and non-biomass
In addition to the synergistic pelletizing of two biological substrates,
the addition of non-biological substrates for pelletizing has also at-
tracted much scholarly attention. There are many different types of
non-biological substrates, including plant extracts, organic synthetics,
production waste, minerals, etc. The advantages of good pelletization,
high economy and waste utilisation can be achieved by adding such sub-
stances. Compared to the addition of biobased material for pelletizing,
this expands the range of additives available and makes the best of local
resources. Table 5 shows the status of research on several non-biological
substrate additive pellets.
Some sugar extracted from plants such as starch and cellulose can
improve the physical quality of the pellets. It facilitates the bonding
between raw material pellets during pelletizing, thus improving the
strength and durability of pellets. In addition, sugar has a high calorific
value and is free of ash and N and S elements, and its addition can im-
prove the combustion characteristics of the fuel (Soleimani et al., 2017).
Starch is a widely used additive, with different types of starch having
different pelleting effects, and some studies have shown that pelleting
properties can be improved by adding maize starch (Razuan et al., 2011,
Ståhl et al., 2012). The addition of oxidised starch and natural starch to
pellets also has different effects on the pellets. Ståhl et al (Ståhl et al.,
2012) found in their study of synergistic pelletizing of cedar and starch
that oxidised starch was more beneficial in improving the durability of
pellets than natural starch.
Making full use of industrial or domestic waste and by-products for
biomass pelletizing is economical and environmentally friendly, and fac-
tors such as it having a high calorific value, being conducive to pel-
letizing and improving pelletizing characteristics need to be taken into
account when selecting this type of material. For example, sludge is a
waste product from production and life, which contains a large amount
of energy substances such as sugar and protein, all of which simulta-
neously facilitate the pelletizing of raw materials and improve the pel-
9
Carbon Capture Science & Technology 1 (2021) 100005
letizing quality of the fuel (Ståhl et al., 2012). Waste cardboard and
lignin sulfonate, which are waste and by-products from the paper in-
dustry respectively, have also been added to wood chips for pelletizing
with good pelletizing results (Mediavilla et al., 2012, Lela et al., 2016) .
Glycerol from industrial production is similar to greasy substances and
has a lubricating effect when pelletizing, and its addition in appropriate
amounts helps to reduce the energy consumption of pelletizing.
Sugar and production waste are organic substances with a calorific
value, but experiments have also been conducted to investigate the ef-
fect of inorganic substances on pelletizing, which can mainly improve
the energy consumption and physical properties of pelletized particles.
Song et al (Song et al., 2018) investigated the effect of calcium-based
compounds (CaO, Ca(OH)2) on the pelletizing of oak and sucrose mix-
tures, as sucrose-calcium-based compounds facilitate Lu et al (Lu et al.,
2014) point out that bentonite is viscous and has a lubricating effect,
thus facilitating the bonding of straw pellets and reducing the energy
consumption for pelletizing.
5. Challenges and Perspectives
There is no doubt that biomass pellet fuel is indeed an important
means to transform biomass resources and promote efficient use of
biomass energy. Currently, there are two main types of options for
biopellet upgrading and modification. i) Optimising the operating pa-
rameters of the biopellet pelletizing process (Cui et al., 2019). For ex-
ample, by controlling the temperature, pressure, moisture content and
other operating parameters of matrix materials, combined with response
surface optimization and experimental methods, better biomass pellet
manufacturing parameters were obtained through multi-parameter op-
timisation, aiming at high fuel quality (e.g. pellet density, pellet break-
ing strength, etc.) and low pelletizing energy consumption. With high
fuel quality (such as particle density, pellet crushing strength, etc.),
the pellet energy consumption was low. ii) Matching different types of
biomass from the differences in the internal material composition of dif-
ferent biomass substrate materials for co-pelletizing. As previously dis-
cussed, the use of crops (or waste) containing oil and lipid, sugar, etc.
for co-pelletizing with herbaceous and woody (softwood and hardwood)
crops is beneficial to reducing energy consumption in the preparation of
biomass pellet fuel and improving pellet density and durability. Further-
more, the use of non-biobased materials (domestic production waste,
inorganic additives) for co-pelletizing with biomass also improves the
quality of the pellet fuel and energy consumption to varying degrees.
Although option (i) does improve pellet quality and optimise the pel-
letizing process, it has a limited impact on pellet quality. In contrast, the
co-pelletizing described in option (ii) takes into account the properties
of different materials and allows different materials to be coordinated
with each other in the pelletizing process. As yet, little work has been
reported combining the two options, i.e., optimising the co-pelletizing
process using a multi-parameter multi-objective optimisation approach
to obtain better quality mixed pellets, which appears to be a future re-
search direction.
Furthermore, as co-pelletizing involves different raw materials, the
transport of different materials required for co-pelletizing should be
taken into account when it comes to market applications. According to
Hamelinckya et al (Hamelinck et al., 2005), the transport costs of raw
materials account for 60-75% of their costs. Therefore, the limitations of
the types of raw materials that can be selected due to geographical dif-
ferences needs to be taken into account. In addition, the use of advanced
biomass resources such as microalgae for co-pelletizing with wood and
herbs seems to be a current direction worthy of further research, i.e.
the use of industrial flue gas to cultivate microalgae and the photo-
synthesis of microalgae for efficient CO2 fixation in photobioreactors
(Xuyang et al., 2021). The obtained microalgae are then co-pelletized
with conventional biomass (e.g. wood) to prepare the obtained algal
solid biofuel (Cui et al., 2019). This fuel can be mixed and co-combusted
with other fuels, such as coal, to provide a constant amount of electri-
X. Cui, J. Yang, Z. Wang et al. Carbon Capture Science & Technology 1 (2021) 100005

Table 5
Research on biomass-non-biomass co-pelleting

Type of synergy Raw materials Impact Ref.

Sugars Palm kernel cake + corn
starch, tapioca starch and
potato starch
Norway spruce + wheat
starch, corn starch and
potato starch
Spruce, straw + sugar
Straw+Carboxymethylcellulose
Poplar + lignin sulfonate
Industrial or Wood chips + cardboard
domestic waste
Fir, camphor, rice
straw + sludge
Straw + paper sludge
Wood chips + palm oil sludge
Pine wood
shavings + glycerin
Addition of Oak + sucrose-calcium-based
inorganic substances compounds
Straw + bentonite
The mixture of corn starch and palm kernel cake has the most significant (Razuan et al., 2011)
improvement on pelleting quality. When the corn starch content is 10%, the
pellet strength reaches the maximum and the density increases slightly.
The addition of starch leads to a decline the energy consumption of (Ståhl et al., 2012)
pelletizing but an increase in the durability of pellet. In addition, oxidized
starch has a more pronounced improvement effect than natural starch, and
the addition of oxidized corn starch has the best effect.
Sugar substances have a high calorific value and do not contain N, S (Soleimani et al., 2017)
elements or ash. In addition, fructose pelletizes best with spruce and
molasses with straw, both of which are beneficial to increasing the
durability of pellets.
When carboxymethyl cellulose was mixed with cotton and wheat straw, (Si et al., 2016)
hydrogen bonds were formed between the two, and also a solid bridge-like
connection was formed, thus improving the quality of the pelleted particles
and reducing the energy consumption for pelletizing.
Lignin sulfonate is a by-product of the paper industry, and lignin sulfonate (Mediavilla et al., 2012)
makes the surface of pellets smooth and crack-free while reducing the
energy consumption of pelletizing.
Cardboard waste mixed with wood chips is more economical for pelletizing, (Lela et al., 2016)
while the expansion density and strength of pellets are enhanced by adding
cardboard, but the calorific value decreases and the ash content increases.
Sludge contains a large amount of protein and sugar. The pelletizing energy (Jiang et al., 2016,
consumption and water absorption can be reduced, but pellet hardness can Zhu, 2014)
be enhanced by mixing sludge with other biomass raw materials.
The rich cellulose of paper sludge improves the quality of pellet, such as (Matúš et al., 2018)
density, hardness, durability and water absorption properties, as well as ash
fusion properties. The optimum amount of paper sludge to be added is
between 10-20 %.
The strength, swelling density, durability and water absorption of the (Obi, 2015)
pelleted pellets were improved after the addition of palm oil sludge, with
the best pelleting results between 30% and 100% palm oil sludge.
In the pelletizing process, 10-20% glycerol is added to play the role of (García et al., 2018)
lubricant, reducing the energy consumption and increasing the energy
density. However, excessive glycerin can degrade the quality of the
particles.
The addition of sucrose improves the strength of pellet, and the addition of (Song et al., 2018,
CaO or Ca(OH)2 improves the effect. This is because the Tu, 2009)
sucrose-calcium-based compounds facilitate the formation of polymers,
while the degradation of sucrose is facilitated under high temperature
alkaline conditions, and the reaction between the degraded products
increases the strength.
Bentonite is a cheap and easily available clay that facilitates the bonding of (Lu et al., 2014)
biomass feedstock and improves the strength of pellets, while also reducing
pelletizing energy consumption.

cal or thermal energy. In this framework, high concentration cultiva-
tion, co-pelleting and co-combustion of microalgae has proven to be
feasible and has great potential for future industrial applications, which
seems to be a new framework for the utilisation of microalgae and CO2
recycling.
6. Conclusion
Based on the perspective of efficient utilisation of biomass pellet fuel,
the influence of the material components of the biomass matrix mate-
rial and the pelletizing operation parameters on the quality of biomass
pellets is reviewed. The components of lignin, cellulose, hemicellulose,
protein, lipids and moisture contained in the raw material are the main
chemical components that influence pelletizing, and different chemical
components have different effects on pelletizing. A single chemical com-
ponent does not determine the pelletizing process. Suitable operating
parameters (e.g. temperature, pressure and suitable moisture content
(generally in the range of 10-12% depending on the type of raw ma-
terial)) also have a significant influence on pelleting, but the influence
of these parameters on pellet quality and pelletizing energy consump-
tion is complex and inter-coupled. For example, biomass richer in lignin
has a higher pelleting temperature; woody plants are easier to pellet
than herbaceous plants and require less energy for pelletizing. In addi-
tion, co-pelleting can be divided into biomass-biomass co-pelleting and
biomass-non-biomass co-pelleting. Common ones are: co-pelletizing of
woody and herbaceous crops; the addition of raw materials with high
starch and oil content to woody or herbaceous crops (e.g. microalgae,
peanut shells, etc.); the mixing of different parts of the same crop (e.g.
bark and leaves of the same quality); co-pelletizing of biomass with solid
waste (e.g. municipal sludge, waste paper scraps, etc.). In conclusion,
considering that the full utilization of biomass is considered as a fa-
vorable option to reduce carbon emissions, the production of biomass
pellet fuel from different types of biomass feedstocks by co-pelletizing
technology is an important and effective option to utilize biomass en-
ergy. Moreover, it has been proven that co-pelletizing can improve the
physical quality (e.g., density, durability) of biomass pellet fuel while re-
ducing pelletizing energy consumption. The economical, environmental
and sustainability of the feedstock are prerequisites for the selection of
co-pelletizing materials.
Credit authorship contribution statement
Xuyang Cui: data curation, writing, original draft preparation, re-
viewing and editing; Junhong Yang: conceptualization, supervision,
writing, original draft preparation, reviewing and editing; Zeyu Wang:
writing, original draft preparation, reviewing and editing; and Xinyu
Shi: original draft preparation, reviewing.

10
X. Cui, J. Yang, Z. Wang et al.
Statement of informed consent, human/animal rights
No conflicts, informed consent, or human or animal rights are appli-
cable to this study.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could appear to influence the
work reported in this paper.
Acknowledgments
This work is supported by the Natural Science Foundation of Tianjin
City, China (No. 13JCYBJC19000).
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