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Fuel 302 (2021) 121076

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Fuel
journal homepage: www.elsevier.com/locate/fuel

Full Length Article

Effect of process parameters and biomass composition on flat-die pellet


production from underexploited forest and agricultural biomass
Simon Lavergne a, b, *, Sylvia.H. Larsson c, Denilson Da Silva Perez d, Muriel Marchand b,
Matthieu Campargue a, Capucine Dupont e
a
RAGT Energie S.A.S., Chemin de la Teulière, 81000 Albi, France
b
CEA Liten, 17 Avenue des Martyrs, 38000 Grenoble, France
c
Swedish University of Agricultural Sciences, Department of Forest Biomaterials and Technology, SE 90183 Umeå, Sweden
d
FCBA, 341 Rue de la Papeterie, 38610 Gières, France
e
IHE Delft Institute for Water Education, Department of Environmental Engineering and Water Technology, Delft, the Netherlands

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

Keywords: This study investigates the impact of biomass moisture content, press-channel length, energy input, and die
Pelletizing temperature on pellet quality in pilot-scale flat-die pellet production. In addition, observed correlations between
Wood pellet pellet quality and the chemical composition of the pelletized biomass assortments are presented. Ten different
Straw
feedstock assortments: Scots pine bark, Scots pine forest residues, willow, poplar stemwood with bark, beech
Bark
Galactose
stemwood with bark, wheat straw, reed canary grass, corn cobs, sunflower shells, and grape seed cakes were
Acetyl groups pelletized in a flat-die pilot-scale pelletizer with a die-channel diameter of 6 mm. The die-channel length varied
within a range of 18–60 mm and biomass moisture content from 10% to 23%. In all, 72 pelletizing experiments
were performed.
Biomass moisture content was the most important parameter for mechanical durability. The feedstock mois­
ture content required to obtain maximum pellet durability depended on the feedstock and showed correlations
with its extractives and galactose content. For all feedstocks, bulk density correlated negatively with moisture
content. The mechanical durability and bulk density of pellets increased with energy consumption. Energy
consumption increased with press-channel length and was correlated with acetyl-group content.

1. Introduction improve processing methodologies. International standards series ISO


17225 [2–4] have been developed to determine several quality classes
Biomass pellets are produced to deliver a product with a high bulk (AX, B, IX) and specifications for woody and non-woody pellets. Physical
density, homogeneous composition, and a particle shape with the requirements are shown in Table 1 and Table 2, and are mainly
following advantages: controlled through the following parameters:

- lower transportation, storage and handling costs; 1) Mechanical durability (DU) is defined as “the ability to withstand
- suitable for automated feeding systems. wear, pressure, or damage and represents the pellets’ resistance to­
wards shocks and/or abrasion as a consequence of handling and
The feeding and particle-shape properties obtained are also benefi­ transportation”. It is expressed in percentage, and quantified by
cial in specific conversion processes, particularly combustion, enabling standard ISO 17831–1:2015 [2]. This parameter is of great impor­
better process control and conversion efficiency [1]. Due to the rising tance because if pellets break during handling and storage, they
global demand for biomass as a feedstock for chemicals, materials, and produce fines that are hazardous for health – inhalation, skin contact
energy, handling and conversion properties are increasingly important. – and safety reasons – self-heating, explosive nature of airborne dust,
Obtaining high pellet quality, especially from unconventional biomasses off-gassing. It can also increase the risk of pellets swelling through
is a challenge, which requires further research and development to

* Corresponding author at: RAGT Energie S.A.S., Chemin de la Teulière, 81000 Albi, France.
E-mail address: simon.lavergne@2016.icam.fr (S. Lavergne).

https://doi.org/10.1016/j.fuel.2021.121076
Received 3 April 2020; Received in revised form 30 March 2021; Accepted 15 May 2021
Available online 2 June 2021
0016-2361/© 2021 Elsevier Ltd. All rights reserved.
S. Lavergne et al. Fuel 302 (2021) 121076

Table 1
ISO 17225–2 physical quality specifications for woody pellets.
Property Unit A1 A2 B I1 I2 I3

Mechanical durability % a.r ≥97.5 ≥96.5 [97.5;99.0] [97.0;99.0] [96.0;99.0]


Fines % a.r ≤1.0 ≤4.0 ≤5.0 ≤6.0
Bulk density kg.m− 3 ≥600
Diameter mm 6–8 6–8-10 6–8-10–14
Length mm [3.15; 40]

3) Specific energy consumption represents the energy needed by the


Table 2 pelletizer to densify a fixed quantity of material. It depends on
ISO 17225–6 physical quality specifications for non-woody pellets.
different process settings (roller- and/or die rotation speed, feeding
Property Unit A B rate, etc.) and on feedstock properties [17]. It has been shown that
Mechanical % a.r ≥97.5 ≥96.0 the energy required to produce biomass pellets has been positively
durability correlated with their physical quality [6].
Fines % a.r ≤2.0 ≤3.0 4) The temperature of the die during pelletizing depends largely on
Bulk density kg.
friction. In industrial production units, die temperature cannot be
≥600
m− 3
Diameter mm 6–8-10–12-25 regulated, but instead reaches an equilibrium [5,15,18–21]. Die
Length mm [3.15; 40] for 6–8-10;[3.15; 50] for temperature (combined with feedstock composition and MC) im­
12–25 pacts softening of natural binding agents in the biomass (lignin and
monosugars). So it is a major factor in pellet quality [10].
moisture sorption, and higher particulate matter emissions from
In the literature, most of the studies of the impact of operating
combustion [1].
conditions have been carried out at laboratory scale, using single-pellet
2) Bulk density (BD) is defined as “the mass of many particles of a
press devices [5,15,18–21]. This type of press only requires a few grams
material divided by the total volume they occupy” and is quantified
of raw material and it is easy to vary operational settings independently
by standard ISO 17828:2015 [3]. It is an important parameter for
from one another. But it is questionable [22] how relevant such results
solid biofuel commercialization because it indirectly represents en­
are to industrial pellet production.
ergy density and gives an idea of the space required for transport and
Furthermore, most of the studies use limited operating conditions.
storage [1].
For example only one moisture content was used: Zamorano et al. [23],
3) The diameter and length of pellets are quantified by standard ISO
with olive wood, almond wood, leaves, black poplar wood and holm oak
17829:2016 [4]. These parameters must be homogeneous, and they
wood; Brand and Jacinto [24] with apple pruning residues; or Lerma-
determine the correct choice of feeding and furnace technology [1].
Arce et al [25] with ten Mediterranean pinewood mixtures.
Systematic studies of different operating settings using a wide range
Pellet quality depends on many parameters, including feedstock
of feedstocks whose compositions are known, under realistic industrial
properties and production conditions [5]. Straws, grasses, and residues
conditions could better control of pelletizing when dealing with new
from forestry and agriculture have been historically used less for
underexploited forest and agricultural biomass. Agar et al. [6] worked in
pelletizing than stem wood and they therefore suffer from a less opti­
this direction by studying pellet production on a ring-die pellet press
mized production technology.
using seven underexploited agricultural and forestry biomasses. This
The lack of process development for these materials entails that they
work yielded unique guidelines for the use of non-conventional feed­
generally have poorer mechanical properties [6,7]. Whittaker and
stock which must be consolidated. An extended analysis of these results
Shield [8] noted that low lignin content and its melting properties, as
has been proposed by Larsson et al [40], which have confirmed by
well as a high extractives content, compared to wood can also explain
Principal Componant Analysis (PCA) that the composition of the feed­
these differences. Castellano et al. [9] and Kaliyan and Morey [10]
stoclss is representative forfor their biomass types: hardwood, softwood
explained that lignin is the most reactive biomass polymer in the auto-
bark, short rotation coppice (SRC), and straw and energy crops. More­
crosslinking reactions occurring in the inter-fiber bonding area of the
over, Orthogonal Partial Least Squares Projections to Latent Structures
particles, and this is responsible for the inter-particle bonding. However,
(OPLS) models were created with the content of macromolecules as
the conditions of lignin softening during pelletizing are still in discussion
factors and pelletizing parameters as responses, which have lead to
[11,12], and consideration of other constitutive elements in pellet
consider acetyl groups, arabinan, xylan, or mannan as new constituents
binding is now suggested [13,14]. which requires further research.
with a probable impact on pelletizing moisture content and press
In industrial production, four main operating conditions impact
channel length used for producing high durability pellets.
pellet quality:
The objective of the present study is to systematically analyze the
links between biomass composition for ten different biomass assort­
1) Moisture improves the bonding between particles but also reduces
ments; five from forestry and five from agriculture, to varying combi­
friction in the die due to its lubricating effect. At extreme values,
nations of process settings for a flat-die pelletizer on a relevant industrial
water can create a layer that is too large to hold the particles
scale. Seven of these feedstocks are the same used by Agar et al. [6] and
together. Once an acceptable moisture content has been achieved, it
Larsson et al. [40] and will establish a comparison of the pelletizing
has been shown that higher moisture content (MC) reduces the final
behaviour on another type of pellet press.
BD of the pellet produced; optimal MC, to maximize DU, depends on
To achieve this, we defined the following approach:
the feedstock [8].
2) Press-channel length (PCL) increases friction between biomass par­
1) Produce pellets with a flat die-pelletizer from a wide range of bio­
ticles and channel walls as well as the time during which the material
masses to pinpoint the most suitable moisture content and press-
is exposed to heat and pressure [15]. This parameter must be
channel length for stable production of high-quality pellets.
adjusted according to the compression force required for a specific
2) Identify the effects of moisture content, press-channel length, energy
material [16].
input and die temperature on pellet quality for different feedstocks.

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S. Lavergne et al. Fuel 302 (2021) 121076

Table 3 (screen size: 4 mm) in an industrial hammer-mill (Vertica DFZK, Büh­


Source and collection date of feedstock materials. ler Nordic, Sweden). The visual appearance of the shredded materials is
Label Common name Latin name Place of origin Collection displayed in Fig. 1. After hammer-milling, the materials were shipped to
date RAGT Energie’s laboratory in Albi, France, for pelletizing.
SPB Scots pine bark Pinus sylvestris Hällnäs, Sweden 25/08/2015
FOR Scots pine Pinus sylvestris Robertsfors, 15/09/2015 2.2. Pellet production
forest residue Sweden
SAX Willow (SRC) Salix ssp. Enköping, Djurby 04/11/2015 Pelletizing and sampling were carried out according to the proced­
gård, Sweden
POC Poplar chips Poplar ssp. Toulouse, France 28/07/2016
ures described in Fig. 2. For each experimental setting, 10 kg of milled
BEC Beech chips Fagus ssp. Toulouse, France 28/07/2016 material was conditioned by adding water to a mixer operating for at
WST Wheat straw Triticum ssp. Mälardalen, 01/10/2015 least 20 min to obtain even moisture. The conditioned material was then
Sweden fed into a 50L silo and conveyed by a screw feeder into a 3 kW flat-die
RCG Reed canary Phalaris Umeå, Sweden 01/05/2010
pelletizer (14–175, Amandus Kahl, Germany) (Fig. 3).
grass arundinacea
CCB Corn cobs Zea mays Rodez, France 16/10/2015 The pelletizer has two rollers (130 mm; width, 29 mm) over a flat die
SFS Sunflower Helianthus Bassens, France 16/10/2015 (175 mm; 6 mm channels with lengths of 6, 12, 18, 21, 24, 27, 30, 33,
shells annuus 36, 42, 48, 54, 60, 72, or 84 mm). The pellets are cut by knives set 25
GSC Grape seed Vitis vinifera Beziers, France 28/10/2015 mm from the die outlets. After pelletizing, pellets are cooled on 3.15 mm
cakes
sieves at ambient temperature. Pelletizer motor current (A), electric
frequency (Hz), power (kW), motor angular velocity (rpm) and die
3) Discuss the influence of biomass composition and settings on flat-die temperature (◦ C) were recorded continuously (1 Hz) with a data logging
pellet production process behavior and pellet quality and compare it system (SIMATIC WinCC, Siemens, Germany).
with corresponding results from the Agar et al. [6] and Larsson et al. Due to the different MC and PCL ranges for obtaining acceptable
[40] studies. pellet quality and production behavior, an experimental design with
identical settings for all feedstock assortments was not feasible. The
ranges for PCL and MC for each specific material were determined by
2. Materials and methods
pre-trials to obtain a good pellet shape, low fines and a reasonable
production rate. Based on these pre-trials, pelletizing was performed at
2.1. Biomass materials
the setting combinations presented in the appendix (Table A).
Before each run, the chosen die was warmed up to 80 ◦ C by pellet­
Five forestry and five agricultural biomasses represented both
izing olive pomace or walnut. Then, two samples of the studied mixture
Northern and Southern European climatic zones, were selected with
were collected and their moisture content was determined according to
regard to their potential for use as solid biofuel. Beech (Fagus ssp.) and
the oven-standard method [26]. Pelletizing was performed at a nominal
poplar (Poplar ssp.) stem wood with bark, corn (Zea mays) cobs, sun­
power consumption of 3 kW. Once production was stabilized, generally
flower (Helianthus annuus) shells and grape (Vitis vinifera) seed cakes
after at least 10 min, measurements started, and two different samples
were collected in France. Scots pine (Pinus sylvestris) bark and forest
were collected in plastic containers for 120 s. All pellets produced during
residues, willow (Salix ssp.), wheat (Triticum ssp.) straw, and reed canary
this time were cooled until the following day. Sampled pellets were
grass (Phalaris arundinacea) originated in Sweden. The source and
weighed to measure the production flow rate (kg/h) and sieved (screen
collection date of these feedstocks are displayed in Table 3. All feed­
size: 3.15 mm) to determine the amount of fines (%). Finally, three
stocks were prepared at the Biomass Technology Centre (BTC) in Umeå,
samples were collected from the total quantity produced during the test
Sweden, where they were dried at 40 ◦ C with a flatbed dryer and
and analyzed for mechanical durability (%) and bulk density (kg/m3).
shredded (screen size: 15 mm) in an industrial shredder (Micromat
2000, Lindner-Recyclingtech GmbH, Austria) and hammer-milled

Fig. 1. Shredded feedstocks. From left to right from above: a) Scots pine bark; b) Scots pine forest residues; c) willow; d) poplar stemwood with bark; e) beech
stemwood with bark; f) wheat straw; g) reed canary grass; h) corn cobs; i) sunflower shells; j) grape seed cakes.

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S. Lavergne et al. Fuel 302 (2021) 121076

Table 4
Higher and lower heating value, ash content and ultimate analysis (wdb =
weight-% dry basis).
Parameter HHV LHV C H O N S Cl
Standard ISO ISO 16948:2015 ISO 16994:2016
18125:2017
Unit MJ.kg− 1 %wdb %wdb

Scots pine bark 20.8 19.7 52.5 5.7 38.6 0.4 0.03 0.08
Scots pine 20.6 19.4 51.2 6.0 40.0 0.7 0.03 <0.01
forest
residues
Willow 18.4 17.2 48.6 5.9 42.7 0.5 0.03 <0.01
Poplar 18.0 16.7 49.0 5.9 43.5 0.2 <0.10 –
stemwood
Beech 18.2 16.9 49.1 6.0 43.0 0.2 < –
stemwood 0.10
Wheat straw 18.9 17.8 44.6 5.6 39.9 0.5 0.13 0.46
Reed canary 18.9 17.6 47.4 5.9 39.4 0.7 0.08 0.06
grass
Corn cobs 18.5 18.0 47.4 6.1 44.3 0.4 0.03 0.14
Sunflower 20.2 18.9 51.5 6.3 38.2 0.8 0.09 0.04
shells
Grape seed 20.4 19.2 50.6 5.8 36.8 2.5 0.16 <0.01
cakes

in [34] by ASE (Accelerated Solvent Extractor) type extraction in two


cycles at 1500psi, firstly with water at 110 ◦ C, then with acetone at
95 ◦ C. Solvents were evaporated under reduced pressure, and the resi­
Fig. 2. Pellet production and sampling procedures. MC = moisture content;
dues were weighed and reported as the extractive content. Acetyl groups
PCL = pellet die channel length.
were analyzed with an internal method detailed in [34] by ion chro­
matography with an IonPac AS11.HC column and an electrometric de­
2.3. Characterization of feedstock and pellets tector in conductometric mode with an eluent gradient NaOH 60 mM
and water.
2.3.1. Feedstock Higher (HHV) and lower (LHV) heating values, and CHON, S, and Cl
Chemical analysis of the milled and dried materials was carried out contents for each feedstock are presented in Table 4, cellulose and
at FCBA, Grenoble, France, using standard methods [27 28 29 30 31 32 hemicelluloses, lignin, extractives, and ash contents in Table 5, glucose,
33]. Extractives were analyzed according to an internal method detailed xylose, mannose, galactose, arabinose and acetyl groups content as a

Fig. 3. Pelletizer design detailed with picture of rollers and flat die.

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S. Lavergne et al. Fuel 302 (2021) 121076

Table 5
Macromolecular composition (wdb = weight-% dry basis).
Parameter Cellulose Hemicellulose. Lignin Extractives Ash Mass balance
Standard TAPPI T249 cm-85 TAPPI T222 om-83 & 4 Internal method ISO 18122:2015 Calculation
Unit %wdb

Scots pine bark 21.9 18.3 40.7 15.2 2.8 98.9


Scots pine forest residues 22.3 27.9 27.5 18.9 2.2 102.3
Willow 44.3 22.6 25.1 8.0 2.8 98.5
Poplar stemwood 42.7 21.8 26.9 4.4 2.8 98.5
Beech stemwood 41.3 25.3 26.5 1.9 0.8 95.7
Wheat straw 38.1 24.7 22.4 7.8 9.3 102.3
Reed canary grass 39.5 25.7 24.7 6.4 6.6 102.8
Corn cobs 38.4 34.8 15.9 6.9 1.9 97.7
Sunflower shells 37.0 26.4 25.9 10.7 8.3 105.9
Grape seed cakes 7.8 21.9 62.8 7.6 4.2 104.2

Table 6
Neutral monosugar distribution and functional groups of feedstocks (wdb = weight-% dry basis).
Parameter Glucose Xylose Mannose Galactose Arabinose Acetyl groups
Standard ASTM E1758 Calculation
Unit % of total monosugars %wdb

Scots pine bark 64.3 7.9 9.9 7.1 10.9 1.6


Scots pine forest residues 58.8 10.7 14.4 8.7 7.5 2.7
Willow 69.1 21.8 2.8 3.0 3.4 4.9
Poplar stem wood with bark 68.9 22.7 4.3 2.0 2.2 5.9
Beech stem wood with bark 63.9 29.1 3.0 2.0 2.0 8.3
Wheat straw 61.0 32.5 0.3 1.6 4.6 3.7
Reed canary grass 61.0 29.9 0.4 3.1 5.6 5.0
Corn cobs 52.4 39.4 0.0 2.5 5.7 5.0
Sunflower shells 59.5 30.7 1.0 2.2 6.6 7.5
Grape seed cakes 33.6 48.2 7.4 5.2 5.6 3.1

percentage of the total amount of monosugars in Table 6. 2.4. Data exploitation for measuring the effect of biomass composition

2.3.2. Pellet quality Mechanical durability was considered the most important parameter
Mechanical durability [2], bulk density [3], and pellet diameter and for assessing pellet quality: it is the best indication of the risk of pellet
length [4] were analyzed as recommended in the solid biofuel standards. deterioration and fines production during transport and handling. It is

Fig. 4. A) Mechanical durability and C) bulk density as a function of feedstock moisture content when using the die-channel length yielding the highest pellet
durability. B) Mechanical durability and D) bulk density of pellets as a function of press-channel length, at the feedstock moisture content that provided the highest
pellet durability.

5
S. Lavergne et al. Fuel 302 (2021) 121076

Fig. 5. A) Mechanical durability, C) bulk density as a function of energy input; and B) mechanical durability, and D) bulk density of pellets as a function of die
temperature when using the die channel length yielding the highest pellet durability.

also the most difficult parameter to maximize during production. So Pellet BD decreased with increasing MC for all feedstocks except
more detailed analysis was carried out to optimize this parameter. For beech (Fig. 4. C.). The moisture effect was most pronounced for Scots
each feedstock assortment, two replicate runs at the setting that pro­ pine forest residues and wheat straw.
duced pellets with the highest mechanical durability were performed,
and averages for the data obtained from these three tests were 3.2. Press-channel length
calculated.
Linear regression models for each pellet quality and process pa­ PCL had a significant positive correlation with pellet DU for corn
rameters versus the physicochemical properties of feedstock were cobs, sunflower shells, forest residues, reed canary grass, willow, and
created, with coefficients of determination (R2) to evaluate their po­ beech, in descending order. No significant effect was found for Scots
tential connections. pine bark, poplar, and wheat straw (Fig. 4. B.).
PCL had a positive effect on BD for all feedstock assortments. The
3. Results magnitude of the effect increased in the following order: Scots pine bark,
wheat straw, Scots pine forest residues, poplar, reed canary grass, beech,
Process settings and pellet properties for each test are presented in corn cobs, and sunflower shells (Fig. 4. D.).
the appendix (Table A). Batches yielding the highest DU are highlighted.
High pellet qualities were obtained from most of the feedstocks. The 3.3. Energy input
highest DU and BD values were obtained with sunflower shells, the
lowest DU with beech, and the lowest BD with wheat straw. Energy had a positive correlation with pellet DU for beech and poplar
The effects of feedstock moisture content (MC), press-channel length (Fig. 5. A). For Scots pine barks, corn cobs and sunflower shells, pellet
(PCL), energy input (E), and die temperature (DT), on pellet durability DU was not affected by changing E, whereas for Scots pine forest res­
(DU) and bulk density (BD) are presented below. idue, willow, wheat straw, and reed canary grass pellet DU varied with
no change in E.
3.1. Moisture content If we exclude beech, which behaved in a very particular way during
pelletizing due to the high MC required, it seems that a general trend
To obtain pellets of reasonably high quality, pelletizing was per­ emerged independently of the feedstock considered: at high E values,
formed at pre-determined MC intervals. Most feedstock could be above 90kWh/T, high DU readings were obtained; for low E, below
pelletized in the 12–16% MC interval, but Scots pine forest residues 70kWh/T, lower DU values were obtained.
required a 10–14% MC interval to obtain good pellets, and wheat straw E had a positive correlation with pellet BD for Scots pine residue, and
and beech a 18–22% MC interval (Fig. 4. A). MC was negatively corre­ a negative correlation for willow, reed canary grass, and poplar (Fig. 5.
lated with pellet DU for Scots pine forest residues. Willow and poplar C). Decreasing BD could be explained by the fact that increasing E was
pellet DU increased with higher MC values up to approximately coupled with increased moisture content. No significant effect was
14–15%. Beech pellet DU increased with MC in the 18–22% range. No found for beech, corn cobs, and sunflower shell. No change in energy (E)
significant effect of MC on DU was observed for the other assortments. was observed for Scots pine forest residue and wheat straw, whereas

6
S. Lavergne et al. Fuel 302 (2021) 121076

Fig. 6. A) Pelletizing moisture content of batches with best durability as a function of extractives, and B) galactose content. C) Press-channel length content of
batches with best durability as a function of soluble lignin content. D) Energy input for batches with best durability as a function of acetyl groups content.

their apparent density (BD) did vary. “optimum MC” values were specific to the feedstock used.
Again, if we exclude beech, a general trend is apparent indepen­ This optimum MC was negatively correlated with extractive content
dently of the feedstock considered: a high E value could yield high BD. (Fig. 6 A), mainly due to the high level of extractives coupled with low
However, this is less clear than for DU due to the combined effect of optimum MC for Scots pine bark and forest residues and the low level of
moisture content on BD. extractives at a high optimum MC for beech.
In the literature, extractives were seen as causing a fall in both pellet
3.4. Die temperature durability and energy input, due to the formers’ lubricant effect on press
channels [35]. At the same time, moisture is also thought to have a
Reasonably high quality pellets were obtained in a range of lubricant effect during pelletizing [6]. This may explain why lower MC is
95–115 ◦ C for all pellets except Scots pine forest residue pellets, which required when feedstocks contain a higher extractives level, competing
were produced in a range of 80–95 ◦ C (Fig. 5. B). DT had no significant in this situation.
effect on DU. Some authors have also suggested that extractives may block binding
DT had a negative correlation with pellet BD for wheat straw and sites for hydrogen bonding during pelletizing [36], which would reduce
reed canary grass (Fig. 5. D). No significant correlation was found for the importance of water in activating natural binders. Larsson et al. [40]
Scots pine bark, willow, poplar, beech, corn cobs and sunflower shells. found a negative correlation between water-soluble extractives and
pelletizing moisture content used in ring-die pellet production with
4. Discussion similar materials.
Optimum MC was also negatively correlated with the galactan con­
Maximum pellet mechanical durability and the corresponding bulk tent of feedstocks (Fig. 6 B), mainly due to the high level of galactan
density were not correlated with any feedstock component. coupled with low optimum MC for Scots pine bark and forest residues.
The lignin content, considered as an essential constituent for Frodeson et al. recently showed that there is variation in how the
pelletizing biomasses [10] did not lead to higher DU contrary to what polysaccharides are affected by changes in MC [37]. Galactose was
Whittaker & Shield [8] or Castellano et al. [9] found. As discussed by treated as one of the “other polysaccharides“ and it has been suggested
Zeng et al [11], the softening mechanisms of lignin are heterogeneous that its moisture may have influenced its thickening effect during
depending on the biomass, and the temperature ranges where good pelletizing. Larsson et al. [40] have found that the distribution of xylan
densification occurs may not have been reached in all cases. and mannan in the feedstock affected the optimum moisture content in
Cellulose and hemicelluloses, seen as affecting the binding mecha­ ring-die pellet production. They hypothesized that this is due to dis­
nisms of lignin by Jiang et al. [17], were correlated to neither maximum similarities in these hemicelluloses’ comparably high, sorption capac­
pellet DU nor the corresponding BD. ities which, in turn, have a marked impact on the biomasses’ softening
The diversity of biomass types and the production method, which behavior.
targeted maximum DU, may explain these differences. In ring-die pelleting, Agar et al. found a negative effect of MC on
pellet BD attributed to the lubricating effect of water [6], but this effect
is more affected by the feedstock type in this study. Again, extractives
4.1. Moisture content
and galactan content could affect the role of water as Scots pine bark,
and forest residues showed the highest negative correlations, whereas
In the interests of industry, the aim was to determine a moisture
beech and corn cobs displayed the lowest negative correlations.
content that resulted in pellets with high mechanical durability. These

7
S. Lavergne et al. Fuel 302 (2021) 121076

4.2. Press-channel length 5. Conclusion

The positive correlation of press-channel length on durability and The aim of this paper was to understand how and why the use of
bulk density is attributed to the increase in the physical forces in the forest and agricultural feedstocks affect production settings and pellet
channel with friction effects as the length increases, leading to greater quality in a real-life production environment.
pelletizing pressure [38]. The results of pelletizing ten different under-exploited feedstocks
In the present study this effect depended on the feedstock in use. were clearly impacted by the material used.
Corn cobs with the lowest lignin and highest hemicellulose content were In general high energy input enhanced durability and bulk density.
the most affected by changes in PCL; Scots pine bark, with the highest Die temperature exerted no observable influence, but pelletizing mois­
lignin and lowest hemicellulose content, was not significantly impacted ture content and press-channel length had to be set to a specific level, its
by changes in PCL. However, wheat straw, with low lignin content, was value and sensitivity depending entirely on the suitable biomass.
not greatly affected by changes in PCL either. Linear regressions showed that the optimal moisture level needed to
As explained previously, this study did not highlight the positive produce high durability pellets was positively correlated with galactose,
impact of lignin on pellet DU contrary to what is commonly suggested in a sugar contained in hemicelluloses, and extractives content. Energy
the literature. These observations may have been made with a sub- input was positively correlated with acetyl group content. Contrary to
optimum PCL, producing low-DU pellets when studying feedstocks what is commonly suggested in the literature, no correlation was found
with low lignin and high hemicellulose contents. between lignin or hemicellulose content and the pelletizing behavior of
The level of PCL needed to obtain the highest pellet DU, called the studied feedstocks. These observations could be explained by the
“optimum PCL”, was only negatively correlated with soluble lignin high diversity of biomass studied here, and further work should be done
content (Fig. 6 C), which was also constatedstated by Larsson et al. [40] to enlarge the number of biomasses and conditions tested or focus on
in ring-die pellet production. On their side, they also found that acetyl biomasses with a specific level of galactose, extractives, or acetyl-group
groups could have a negative impact, which could be due to a reduced content.
hydrophobicity, and that acetone extractives and arabinan could have a From the point of view of pellet producers, Scots pine bark and forest
positive on the PCL, probably because the lubricating effects of these residues could represent the best feedstocks for pelletizing, as produc­
elements requires the application of higher frictional forces. tion resulted in high quality pellets coupled with low energy input and
PCL also affected the impact of MC on DU. At a lower PCL, a variation fines, potentially due to a high level of galactose and extractives, and a
in MC had a greater effect on the durability of willow, corn cobs, sun­ low level of acetyl-group contents. Sunflower shells, corn cobs, and
flower shells and beech pellets. poplar resulted in high-quality pellets but with high energy input.
Hence, choosing a longer press channel could be a good strategy for Grapes seed cakes and reed canary grass resulted in acceptable quality
pellet producers, potentially reducing the risk of variable quality due to pellets and energy input. It was not possible to produce pellets that
moisture flexibility. A compromise needs to be found, as too long a press complied with European quality standards using wheat straw and beech
channel can lead to varying flow rates, hazardous die temperatures, or under the conditions tested in this study.
clogging due to the presence of unexpected frictional forces.
Authorship contributions
4.3. Energy input
Conception and design of study: Simon Lavergne, Sylvia. H. Larsson,
The possible positive correlation of durability and bulk density with Muriel Marchand, Matthieu Campargue, Capucine Dupont. Acquisition
energy may be explained by the fact that pelletizing pressure and E are of data: Simon Lavergne, Sylvia. H. Larsson, Denilson Da Silva Perez.
associated somehow at an industrial scale. Analysis and/or interpretation of data: Simon Lavergne, Sylvia. H.
At the same time, the highest DU for each feedstock was not obtained Larsson, Denilson Da Silva Perez, Matthieu Campargue. Drafting the
with the same E value, or “optimum E”. manuscript: Simon Lavergne. Revising the manuscript critically for
It has been suggested that this value is positively correlated with MC important intellectual content: Simon Lavergne, Sylvia. H. Larsson,
[39] and negatively correlated with extractives content [35]. In the Denilson Da Silva Perez, Muriel Marchand, Matthieu Campargue,
present study, Scots pine bark and forest residue presented low optimum Capucine Dupont. Approval of the version of the manuscript to be
E, associated with low optimum MC and high extractives content; beech published (the names of all authors must be listed): Simon Lavergne,
presented high optimum E, associated with high optimum MC and low Sylvia. H. Larsson, Denilson Da Silva Perez, Muriel Marchand, Matthieu
extractives content, which could confirm this hypothesis. Campargue, Capucine Dupont.
Optimum E was also strongly positively correlated with acetyl group
content (Fig. 6. D). We found no mention in the literature of acetyl
groups having an impact on their own. Further work is needed on the Declaration of Competing Interest
possible impacts of acetyl groups during pelletizing.
The authors declare that they have no known competing financial
4.4. Die temperature interests or personal relationships that could have appeared to influence
the work reported in this paper.
In the literature, die temperature positively affects durability at a
laboratory scale [5]. At pilot scale and using similar feedstock, the Acknowledgments
temperature of pellets measured during extrusion from the die corre­
lated positively with DU and BD [6]. The authors would like to thank Maxime Rojas for his assistance with
The absence of trends in this study could be due to the measurement pelletizing and characterization at RAGT Energie. The authors thank
method. Magnus Rudolfsson and David A. Agar of the Department of Forest
Biomaterials and Technology for discussions and hospitality during the
collaboration. This study was conducted under the EU Horizon 2020
research and innovation programme MOBILE FLIP 637020.

8
S. Lavergne et al. Fuel 302 (2021) 121076

Appendix

Table A.

Table 1A
Process settings, corresponding pellets properties and response parameters of the pelletizer for all feedstocks.
Parameter PCL/D Moisture Durability Bulk density PelletM. C. Pellet Fines Die Energy
content production production temperature input
Standard - IS/TC 238 ISO ISO IS/TC 238 - - - -
17831–1:2015 17828:2015
Unit mm % % kg/m3 % kg/h % ◦
C kWh/T

Scots pine barks 48/6 12,0 0,0 98,2 0,1 708 0 9,0 0,0 52 10 0,6 0,5 101 5 61 10
Scots pine barks 48/6 13,1 0,0 98,1 0,1 700 0 9,8 0,0 56 3 0,4 0,2 103 5* 51 2
Scots pine barks 48/6 14,7 0,1 98,2 0,0 681 2 10,9 0,1 63 2 0,4 0,0 96 5* 46 2
Scots pine barks 36/6 12,0 0,0 97,8 0,1 694 4 9,2 0,0 57 1 0,8 0,3 90 5* 53 2
Scots pine barks 36/6 13,1 0,0 97,8 0,0 682 0 9,6 0,0 63 4 0,7 0,3 100 5* 45 2
Scots pine barks 36/6 14,7 0,1 97,7 0,1 660 1 10,8 0,1 52 22 0,4 0,2 90 4 69 32
Forest residue 48/6 10,7 0,1 97,0 0,3 614 1 8,9 0,7 63 1 0,1 0,0 91 1 48 2
Forest residue 48/6 11,4 0,2 95,0 0,0 550 1 10,0 0,0 68 5* 0,2 0,3* 82 2* 44 3*
Forest residue 48/6 14,4 0,2 93,0 0,1 469 1 11,4 0,0 65 5* 0,5 0,3* 85 2* 49 3*
Forest residue 42/6 10,7 0,1 93,7 0,6 584 3 8,4 0,7* 71 5* 0,3 0,3* 82 2* 44 3*
Forest residue 42/6 11,0 0,2 92,9 0,0 560 2 8,7 0,7* 70 5* 0,2 0,3* 83 2* 41 3*
Forest residue 42/6 14,3 0,2 87,3 1,2 463 2 11,6 0,2 72 5 0,4 0,3 78 2 40 3
Willow 42/6 10,3 0,0 95,3 0,0 674 2 7,1 0,1 48 1* 0,0 0,0* 96 1* 61 1*
Willow 42/6 12,0 0,0 98,2 0,1 660 1 8,8 0,0 48 1* 0,0 0,0* 95 1* 60 1*
Willow 42/6 14,2 0,0 99,1 0,1 643 6 10,6 0,3 48 1* 0,1 0,0 99 1 62 1*
Willow 42/6 15,2 0,3 98,7 0,0 636 1 11,0 0,1 50 1* 0,0 0,0* 97 1* 61 1*
Willow 42/6 16,5 0,0 98,5 0,2 635 3 11,9 0,1 46 1* 0,0 0,0* 100 1* 66 1*
Willow 42/6 18,3 0,0 99,1 0,0 593 2 12,5 0,0 42 1* 0,0 0,0* 96 1* 72 1*
Willow 42/6 20,5 0,0 99,0 0,0 572 2 15,0 0,1 39 1* 0,0 0,0* 98 1* 77 1*
Willow 33/6 10,3 0,0 90,2 0,5 603 2 7,5 0,0 56 1* 0,0 0,0* 91 1 46 1*
Willow 33/6 12,0 0,2 95,4 0,3 597 3 8,7 0,2 59 1* 0,0 0,0* 92 1 45 1*
Willow 33/6 14,2 0,0 96,1 0,3 554 0 11,2 0,1 49 1* 0,1 0,0* 95 1* 59 1*
Willow 33/6 15,2 0,3 96,1 0,3 561 31 11,2 0,0 52 1* 0,2 0,0* 94 1* 52 1*
Willow 33/6 16,5 0,0 96,1 0,2 537 4 11,6 1,0 51 1 0,2 0,0 97 1 58 1
Willow 33/6 18,3 0,0 97,7 0,1 523 5 13,8 0,1 45 1* 0,0 0,0* 96 1* 66 1*
Willow 33/6 20,5 0,0 97,0 0,1 453 5 15,7 0,0 43 1* 0,0 0,0* 100 1* 70 1*
Willow 27/6 10,2 0,0 77,4 2,6 554 4 8,9 0,1 48 1* 0,2 0,0* 94 1* 62 1*
Willow 27/6 12,6 0,1 87,1 1,5 537 2 10,2 0,1 58 1* 0,1 0,0* 92 1* 52 1*
Willow 27/6 14,9 0,3 94,4 0,6 524 8 11,7 0,0 56 1* 0,0 0,0* 94 1* 54 1*
Willow 27/6 15,9 0,1 94,5 0,4 520 10 11,5 0,1 54 1* 0,0 0,0* 94 1* 57 1*
Willow 27/6 16,7 0,2 94,7 1,5 505 5 12,2 0,0 50 1* 0,0 0,0* 95 1* 59 1*
Willow 27/6 18,5 0,3 96,5 0,2 488 12 13,3 0,1 43 1* 0,0 0,0* 95 1* 69 1*
Willow 27/6 21,6 0,3 89,4 6,7 394 10 15,3 0,1 38 1* 0,0 0,0* 96 1* 80 1*
Poplar chips 42/6 12,2 0,1 95,7 0,0 712 1 7,1 0,1 38 1 0,1 2,4* 112 2* 78 14*
Poplar chips 42/6 14,7 0,0 98,6 0,1 690 1 8,2 0,1 34 1 0,1 2,4* 111 2* 85 2
Poplar chips 42/6 16,8 0,1 98,9 0,1 685 8 9,4 0,5 32 3 1,3 1,1 114 2 91 7
Poplar chips 33/6 12,2 0,1 95,0 0,2 684 5 7,5 0,3 37 3 2,9 2,4 110 2 80 8
Poplar chips 33/6 14,7 0,0 98,4 0,1 668 2 8,7 0,0 36 5 0,2 2,4* 110 2* 82 12
Poplar chips 33/6 16,7 0,0 98,9 0,1 639 2 10,5 0,1 38 7 0,2 2,4* 109 2* 78 14
Beech chips 30/6 18,5 0,1 95,8 0,9 645 2 7,4 0,1 24 1 0,2 0,0 113 1 133 8
Beech chips 30/6 20,8 0,1 96,5 0,8 675 2 7,9 0,1 21 1* 0,0 0,0* 107 4* 148 8*
Beech chips 30/6 23,0 0,1 96,8 0,3 611 3 7,6 0,0 19 1* 0,0 0,0* 110 4* 156 8*
Beech chips 18/6 18,1 0,3 93,6 0,4 515 1 10,6 0,5 33 1 3,1 5,3 104 4 96 2
Beech chips 18/6 20,8 0,2 86,7 0,6 403 0 12,0 0,0 33 1* 5,8 5,3* 96 4* 91 8*
Beech chips 18/6 22,1 0,2 58,0 0,3 336 1 11,2 0,0 32 1* 4,6 5,3* 97 4* 93 8*
Wheat straw 48/6 18,5 0,0 97,1 0,1 552 1 12,3 0,7 40 6 0,9 0,9 98 2 57 6
Wheat straw 48/6 19,8 0,7 96,6 0,2 543 3 – – 35 6* 0,3 0,9* 100 2* 68 8*
Wheat straw 48/6 20,7 0,2 97,2 0,1 502 2 13,5 0,0 32 6* 0,2 0,9* 102 2* 69 8*
Wheat straw 42/6 18,0 0,0 97,2 0,1 535 1 12,3 0,1 32 6* 0,2 0,9* 94 2* 57 8*
Wheat straw 42/6 19,8 0,7 95,0 0,5 509 0 13,2 0,0 22 6* 0,4 0,9* 96 2* 89 8*
Wheat straw 42/6 20,7 0,2 95,1 0,3 463 6 14,0 1,2 33 4 1,0 0,7 97 0 64 8
Reed canarygr. 48/6 13,3 0,2* 96,8 0,0 713 5 8,9 0,1 – – – – 98 3* – –
Reed canarygr. 48/6 14,0 0,0 97,0 0,1 701 2 10,2 0,0 38 2* 5,4 2,0* 99 3* 64 4*
Reed canarygr. 48/6 15,0 0,1 96,4 0,2 693 2 10,6 0,1 39 2* 1,3 2,0* 101 3* 68 4*
Reed canarygr. 48/6 15,9 0,1 98,2 0,2 675 4 11,6 1,2 40 2 0,9 0,1 102 1 67 3
Reed canarygr. 42/6 13,1 0,2* 91,3 0,6 662 6 9,5 0,1 26 2* 5,6 2,0* 98 3* 81 4*
Reed canarygr. 42/6 14,0 0,0 92,2 0,9 636 3 10,4 0,4 48 1 6,1 2,0 95 3 56 4
Reed canarygr. 42/6 15,1 0,1 93,7 0,1 634 2 10,8 0,0 50 2* 3,0 2,0* 98 3* 58 4*
Reed canarygr. 42/6 16,2 0,2 95,8 0,4 618 8 11,8 0,1 50 2* 5,6 2,0* 100 3* 55 4*
Corn cobs 27/6 12,1 0,0 99,1 0,0 699 0 6,1 0,1 31 5* 0,1 0,0* 107 4* 94 8*
Corn cobs 27/6 14,1 0,3 99,2 0,1 704 0 7,7 0,5 31 3 0,1 0,0 111 4 100 8
Corn cobs 27/6 16,5 0,1 99,3 0,0 685 0 8,4 0,0 25 5* 0,2 0,0* 105 4* 122 8*
Corn cobs 18/6 12,3 0,3 83,9 2,3 552 0 9,7 0,4 52 5 8,7 2,7 96 4 55 3
Corn cobs 18/6 14,0 0,0 68,8 0,3 469 0 11,1 0,1 53 5* 9,8 2,7* 89 4* 54 8*
Corn cobs 18/6 16,1 0,0 49,3 0,8 430 0 12,5 0,1 58 5* 9,2 2,7* 82 4* 49 8*
(continued on next page)

9
S. Lavergne et al. Fuel 302 (2021) 121076

Table 1A (continued )
Parameter PCL/D Moisture Durability Bulk density PelletM. C. Pellet Fines Die Energy
content production production temperature input
Standard - IS/TC 238 ISO ISO IS/TC 238 - - - -
17831–1:2015 17828:2015
Unit mm % % kg/m3 % kg/h % ◦
C kWh/T

Sunflower shells 60/6 13,5 0,2 99,2 0,1 724 1 7,3 0,0 30 6* 0,1 0,1* 105 4* 89 5*
Sunflower shells 60/6 14,8 0,0 99,4 0,1 725 1 8,0 0,0 28 6* 0,1 0,1* 105 4* 109 5*
Sunflower shells 60/6 17,1 0,3 99,5 0,0 711 1 8,9 0,0 28 1 0,1 0,0 108 2 109 5
Sunflower shells 48/6 12,9 0,0 76,6 0,2 546 2 11,1 0,0 50 6* 49,2 0,1* 81 4* 60 5*
Sunflower shells 48/6 14,9 0,2 81,4 0,1 506 1 11,9 0,1 79 6* 17,5 0,1* 79 4* 38 5*
Sunflower shells 48/6 16,5 0,1 87,3 0,1 475 6 13,1 0,0 83 6 4,9 0,1 82 4 36 4
Grape seeds cake 30/6 16,1 0,1 95,9 0,3 671 5 12,3 0,1 54 3 3,7 0,7 97 1 55 3

*estimated

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