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Article history: Pelletization has been widely used for mass and energy densification of biomass. As the demand for pel-
Received 14 May 2016 lets increases, the conventional raw materials will be insufficient. In this study, the feasibility of sludge
Received in revised form 16 July 2016 mixed with biomass pellets as a solid fuel was researched. Sludge mixed pellets and pure biomass pellets
Accepted 15 August 2016
were investigated to evaluate the energy consumption and pellet properties, including proximate
analysis, moisture adsorption, pellet density, Meyer hardness, volume expansion, higher heating value
and combustion characteristics. The results showed that sludge mixed pellets had reduced energy input,
Keywords:
increased hardness, decreased moisture absorption rate and improved combustion characteristics
Sewage sludge
Biomass
compared with pure biomass pellets. However, the increased ash content of sludge mixed pellets should
Pelletization be noted. These results indicate that there is a balance between an improvement in fuel quality and an
Energy consumption increase in ash content. The sludge mixed pellets could be a suitable solid fuel.
Combustion characteristics Ó 2016 Elsevier Ltd. All rights reserved.
1. Introduction preferred raw materials for wood pellet production, such as cutter
shavings and sawdust, are consumed to the maximum extent. This
Currently, renewable energy developing has received consider- results in the highly competitive raw material market among pellet
able attention in the world. Among these renewable energies, den- making, fired power generation, charcoal, and plate industries. The
sified biomass, especially pellets has drawn the global attention competitive raw material market has been increasing the price of
due to its advantage over raw biomass such as its physical and raw material. In recent years, various biomass materials had been
combustion characteristics [1]. In China, densified biomass fuel used to make pellets, such as tea waste, bamboo, waste paper and
was sought by the government to replace coal in present firing wheat straw mixtures, switchgrass, cotton stalk, rapeseed cake,
plants without any significant modifications because of the rapid olive cake, palm kernel cake, corn stover, reed canary-grass, peanut
growth of energy demands and the dwindling reserves of fossil fuel hulls and poultry litter [7–10]. However, it is not enough at all with
[2]. The production capacity of pellets using agriculture wastes in the development of pellets industry. On the other hand, the
China was 3 million ton in 2010, and aimed to increase to mechanical strength and hardness of pellets made from the above
10 million ton in 2015, furthermore reach to 50 million ton by biomass were always unsatisfactory as mixing unknown biomass
the year of 2020 [3,4]. for pelleting procedure. The addition of binders can improve the
The primary biomass materials used for making pellets are not mechanical strength. However, higher price of binder increased
only wood residues, such as sawdust, wood shavings and wood the feedstock cost of pelletization.
chips, but also agro-residues, such as straw, waste products of Sewage sludge (SS) is a complex heterogeneous mixture of
the food industry and fuel crops [5,6]. Meanwhile, the pellet microorganisms, inorganic materials, moisture and undigested
markets have developed fast in the past decade. Therefore, the organics including paper, plant residues, oils, or fecal material.
Conventional sludge disposal methods including landfill, incinera-
⇑ Corresponding authors at: College of Environmental Science and Engineering, tion, ocean disposal and land application are already facing
Hunan University, Changsha 410082, PR China (X. Yuan). increasing pressure and protest from environmental authorities
E-mail addresses: yxz@hnu.edu.cn (X. Yuan), tcuhui@gmail.com (H. Li). and from the public domain [11]. It is known that SS contains a
http://dx.doi.org/10.1016/j.enconman.2016.08.035
0196-8904/Ó 2016 Elsevier Ltd. All rights reserved.
510 L. Jiang et al. / Energy Conversion and Management 126 (2016) 509–515
significant amount of proteins and carbohydrates, which could materials was analyzed by CHNOS Elemental Analyzer Vario EL
serve as a potential natural binder to make it suitable for pelleting III (Elementar Analysen systeme GmbH, Germany). Proximate
[12]. Dospoy et al. [13] firstly managed to produce sludge derived analysis was carried out according to the Standard Practice for
fuel from paper sludge, powder coal, and plastics and realized the the Proximate Analysis of solid biofuels (GB/T28731-2012) using
industrial application. Currently, several studies have been con- a Jinghong SXL-1002 program control chamber electric furnace
ducted, focusing on the physical properties and combustion char- (China). The higher heating value (HHV) was determined using
acteristics of sludge refuse-derived fuel (RDF) [14–18]. However, an oxygen bomb calorimeter (SUNDY SDACM5000, China) from
the feasibility of sludge mixed with biomass to produce pellets three replicates. The amounts of cellulose, hemicellulose and lignin
using a single pellet press and the effect of sludge addition on were obtained using Van Soest detergent fiber analysis by
the energy consumption and pellet properties have never been automated fiber extraction analyzer (Gerhardt fibretherm FT12,
reported. The results of this study are significant for the feasibility Germany). Protein was calculated by multiplying the concentration
of sludge applying in the current biomass pellet industry. of organic nitrogen by 6.25. Forces and displacement curves in pel-
In this study, three kinds of raw materials (Chinese fir, camphor letization were recorded to calculate the energy consumption. The
and rice straw) were applied for pelletization, representing soft- energy consumptions associated with compaction and extrusion
wood, hardwood and herb, respectively. Sludge mixed pellets and were obtained by integrating the curve. Pellet density was deter-
pure biomass pellets were investigated to compare the energy con- mined by calculating the mass, length, and diameter of pellets.
sumption and pellet properties, including proximate analysis, The volume expansion was calculated by measuring the length
moisture adsorption, pellet density, Meyer hardness, volume and diameter after storing the pellets inside a sealed bottle at
expansion, higher heating value and combustion characteristics. 4 °C for two weeks.
Meyer hardness of pellets was analyzed by the same pellet
2. Materials and methods press unit with a hemisphere-end rod. The Meyer hardness, Hm,
defined as the applied force divided by the projected indentation
2.1. Materials area and was calculated by the following equation [23].
Hm ¼ F=½pðDh h Þ
2
ð1Þ
The sludge was obtained from an urban sewage plant with aer-
obic and secondary treatment in Changsha city, Southern China. where h is the indentation depth (mm); F is the maximum force
Chinese fir (Cunninghamia lanceolata (Lamb.) Hook.), camphor (Cin- when the pellet is broken (N); and D is the diameter of rod (mm).
namomum camphora (L.) J. Presl) and rice straw (Oryza sativa L.) The moisture absorption of pellets was measured in a humidity
were used to represent the class of softwoods, hardwood and grass, chamber (GT-TH-S-150Z, Gaotian, China) setting at 30 °C and 90%
respectively. The elemental and proximate analysis results and relative humidity. Prior to the moisture uptake test, the pellets
some physicochemical parameters of the samples above were were dried in a convection oven at 105 °C for 24 h. The weight of
shown in Table 1. the sample was measured every 10 min at the first hours followed
by every 30 min for the next 4 h. Thin-layer drying formulation as
2.2. Pelletization and characterization of the pellets below was adapted for the kinetic analysis of moisture uptake [24].
M Me
The pellets were prepared using a single pellet press unit which ¼ ekt ð2Þ
Mi Me
allowed simulation of the pelletizing process in a press channel of a
pellet mill [19–22]. Briefly, a cylinder with 7.00 mm in inside where M is the instantaneous moisture content, Me is the equilib-
diameter and 70.00 mm in height with a piston with 6.90 mm in rium moisture content, and Mi is the initial moisture content. The
diameter and 90.00 mm in length was installed for making a single coefficient k is the absorption constant, and t is the exposure time
pellet. The cylinder-piston unit was wrapped by a heating tape (min).
with a thermocouple and a temperature controller to preheat the Combustion characterization of the pellets was carried out by
inside cylinder to a certain die temperature. In this study, the hole thermogravimetric analysis using a thermo-balance DTG-60
of the cylinder was filled with approximately 0.8 g sample to make (Shimadzu, Japan). All combustion experiments were conducted
a single pellet. The sample was pressed by applying a pressure of from room temperature to 800 °C with a heating rate of
83 MPa and held for 30 s. Pure biomass or biomass-sludge mix- 20 °C min1 under an air flux of 100 mL min1. Approximately
tures with a ratio of 50% were used as the samples. The sample 6 mg of sample was used for each experiment.
with 15% moisture content was prepared at 110 °C with the similar
procedure described in a previous publication [23]. 2.3. SEM and UV-AF
The ultimate analysis, proximate analysis, higher heating value,
lignocellulose analysis and protein determination have described Scanning electron microscopy (SEM) and Ultraviolet
in a previous paper [20]. Briefly, the ultimate analysis of the raw auto-fluorescence (UV-AF) were applied to study the bonding
Table 1
Properties of raw sewage sludge and biomass sample.
Analysis Ultimate analysis (d.b. wt%) Proximate analysis (r.b. wt%) Chemical analysis (d.b. wt%) HHV (MJ kg1)
C H N S Moisture Volatile Fixed carbon Ash Protein Hemicellulose Cellulose Lignin
b b
Sludge 36.11 5.25 6.50 1.03 5.42 57.22 6.09 31.27 35.5 – – –b 15.59
Chinese fir 49.08 5.96 0.63 –a 7.63 74.49 16.68 1.20 –b 12.05 36.22 27.61 18.38
Camphor 48.18 6.09 0.70 –a 6.67 79.02 12.53 1.78 –b 20.82 38.87 24.40 18.40
Rice straw 45.04 5.05 1.06 –a 6.56 64.59 13.51 15.34 –b 24.60 41.33 9.22 14.64
mechanism of the prepared pellets by fracture surface analysis. undergoes plasticization. The compression force was initially low
Electron micrographs were recorded using a tabletop microscope for a displacement of 20–40 mm in Region I followed by a rapid
(TM3000, Hitachi Company, Japan) operated at 5–15 kV. UV-AF increase over a relatively short displacement of 5–10 mm in Region
(TE300+Pentamax512EFT, Japan) images of pellet fractured surface II. As shown in Fig. 1, the slopes of the force and displacement in
were obtained to identify the natural binders that coated on the Region II were enhanced with the addition of sludge. Furthermore,
particles [12]. the pure biomass runs experienced a larger elastic compression
than the mixing runs. This might be due to the replacement of bio-
mass with the same amount of sludge which decreased the elastic-
3. Results and discussion ity modulus of material. On the other hand, the protein in sludge
had a synergistic effect with the lignin in biomass [20], thus
3.1. Energy consumption increasing the plasticity of mixed sample during pelletization.
Under the applied pressure and heat, the natural binders (e.g., pro-
There are two energy consumption processes associated with tein, carbohydrate and lignin, etc.) would be squeezed out of the
single pellet producing: compression energy consumption and particles and activated, resulting in the decrement of energy con-
extrusion energy consumption. The compression and extrusion sumption during the compression and extrusion [12]. It was indi-
energy consumptions for Chinese fir pellet (CFP), Chinese fir-SS cated that co-pelletization of sludge and biomass could conduct
pellet (CFSP), camphor pellet (CP), camphor-SS pellet (CSP), rice at low pressure and low temperature compared with pure biomass
straw pellet (RSP) and rice straw-SS pellet (RSSP) were depicted runs [20]. In a word, the sludge used for co-pelletization would
in Table 2. Compression and extrusion energy consumptions of reduce the energy-input cost of pellet production in the plant.
pure biomass pellets were in the following order: CFP > CP > RSP.
It indicated that the energy input in pelletization significantly 3.2. Meyer hardness
depended on the biomass materials and the grass materials needed
less energy consumption. Furthermore, it was found that the The typical breaking force against distance of pure biomass pel-
energy consumption of pure biomass pellets was inversely propor- lets and biomass-sludge mixed pellets are depicted in Fig. 2. The
tional to the content of hemicelluloses in raw biomass. Hemicellu- average value and standard deviation of Meyer hardness for all
loses are the visco-elastic components of wood fiber, which is the pellets are presented in Table 2. As shown in Fig. 2, the force
different from the crystalline structure of cellulose and the amor- and deformation which pellets could withstand were larger after
phous structure of lignin. Therefore, hemicelluloses can introduce adding the sludge. Meyer hardness is one of the important proper-
viscous effect among lignin and cellulose in the fiber [24,25]. The ties of single pellet study, which reflects the strength of pellets dur-
presence of hemicelluloses can reduce the elasticity of particle, ing handling, transportation, and storage. As shown in Table 2, the
and consequently increase the plasticity. In this study, elasticity hardness of biomass-sludge mixed pellets was increased compared
was defined as the resilience characteristics caused by water- with that of pure biomass pellets, such as CFP (3.02 N mm2) and
insoluble fibers which may entangle and fold between particles CFSP (4.15 N mm2). The improvement of hardness for biomass-
or fibers. Plasticity was defined as the viscosity of water-soluble sludge mixed pellets was ascribed to the synergistic effect of pro-
fibers, lignin, protein, starch, fat, and water-soluble carbohydrates. tein in the sludge and lignin in the biomass [20]. The UV-AF images
As shown in Table 2, more energy was needed to make pellets of pellets (Fig. 3) indicated that the natural binders that were
from pure biomass runs than the biomass-sludge mixing runs at coated on the particles in the sludge-biomass mixed pellets were
the same condition (83 MPa, 110 °C and 15% moisture content). primarily lignin and protein [12]. Several studies demonstrated
The compression and extrusion energy for CFSP were 9.8 kJ kg1 that protein played an important role as binding agents
and 0.013 kJ kg1, which were much lower than those of CFP [12,26,27]. Protein denaturation temperature was around 57 °C,
(20.4 kJ kg1, 0.084 kJ kg1). The addition of sludge in the saw- while the lignin softening temperature ranged from 50 to 100 °C
dust/straw can significantly reduce the compression energy, which [28,29]. In the present study, the natural binding components were
may be caused by the smaller fines packing region and the reduced squeezed out of the biomass cells under pressure. After then, lignin
elasticity of material. Two stages are involved during compression and protein were soften or denature in the die temperature
process. The Region I represented the region where the large and (110 °C), improving the structure of hydrogen bonding and solid
small particles were rearranged. The Region II was the plasticiza- bridge between micro-particles of biomass or sludge [12]. The
tion phase of condensed chemical components (e.g., lignin, protein low hardness of biomass pellet may indicate the existence of pore
and carbohydrate) and the second compression phase of the non- spaces and gaps in the pellet which reduces the pellet resistance to
modified chemical components (e.g., cellulose), which occurred deformation. This is confirmed by comparing camphor pellet and
deformation and mechanical interlocking [25]. After the rearrange- camphor-sludge pellet through cross section SEM micrographs
ment of large and small particles, the space between the particles (Fig. 3c and d), in which clear gaps and spaces were identified in
was efficiently filled. Additional force could lead to the initial com- camphor pellets.
pressing phase of particles where the new structure of condensed It was found that several fines (about 1.25%) were separated
chemical components (e.g., lignin, protein and carbohydrate) from the surface of pure biomass pellets after two-week storage,
Table 2
Energy consumptions, Meyer hardness, volume expansion and moisture absorption of raw biomass pellets and their corresponding sludge mixed pellets.
Sample Compression energy Extrusion energy Meyer hardness Volume expansion Equilibrium moisture Absorption rate, k
(kJ kg1) (kJ kg1) (N mm2) (%) content (%) (min1)
CFP 20.4 ± 0.7 0.082 ± 0.009 3.02 ± 0.60 1.33 ± 0.28 15.9 ± 0.5 0.0081
CFSP 9.8 ± 0.3 0.013 ± 0.002 4.15 ± 0.38 0.37 ± 0.19 15.8 ± 0.2 0.0054
CP 18.6 ± 0.3 0.059 ± 0.023 2.87 ± 0.70 1.34 ± 0.29 16.7 ± 0.4 0.0071
CSP 9.8 ± 0.2 0.011 ± 0.001 4.03 ± 0.64 0.57 ± 0.31 16.2 ± 0.2 0.0050
RSP 13.1 ± 0.5 0.028 ± 0.006 3.98 ± 0.16 1.27 ± 0.41 23.2 ± 0.3 0.0041
RSSP 7.2 ± 0.2 0.004 ± 0.001 4.18 ± 0.06 0.31 ± 0.14 19.6 ± 0.1 0.0037
512 L. Jiang et al. / Energy Conversion and Management 126 (2016) 509–515
Fig. 3. UV-Auto-Fluorescence (UV-AF) images and Scanning Electron Microscopy (SEM) images of cross-sections of pellets. The green or yellow-green fluorescence represents
protein compounds. The brilliant blue or bluish-white fluorescence represents lignin. No fluorescence (i.e., black color) may represent cellulose, hemicellulose, starch, water
soluble carbohydrates, and lipid/fat. (a and c) Camphor pellet, (b and d) camphor and sludge pellet. (For interpretation of the references to color in this figure legend, the
reader is referred to the web version of this article.)
B was the main mass loss occurred for biomass pellets due to the
release and burning of volatiles. However, the combustion of
biomass-sludge mixed pellets operated at a more stable way as
the similar mass loss in stage B and stage C. This can be confirmed
by the DTA curves which indicate the detection of thermal effects
accompanied by physical or chemical changes [34]. As shown in
Fig. 6, the DTA curves of biomass-sludge mixed pellets have two
clear thermopositive peaks for volatile burning and char burning.
However, the thermopositive effects of biomass pellets are mainly
from volatile burning at low temperature. Therefore, DTA curves
could explicitly indicate that the combustion of biomass-sludge
mixed pellets operated at a more stable way as the higher ther-
mopositive peaks in stage C.
The characteristic combustion parameters of the pellets are
summarized in Table 4. The ignition temperature was estimated
from the TG and DTG curves according to the method reported
on the literature [14,35]. The final combustion temperature was
defined as the temperature that 99% of the combustible material
Fig. 4. Moisture absorption of raw biomass pellets and sludge-biomass pellets. All has been burnt out [14]. It was clear shown in Table 4 that the
pellets were dried at 105 °C for 48 h before being placed in the humidity chamber biomass-sludge mixed pellets had improved fuel quality than pure
set at 30 °C and 90% RH. biomass pellets, such as reduced ignition temperature (except
Table 3
Proximate analysis, pellet and energy densities of raw biomass pellets and their corresponding sludge mixed pellets.
Sample Moisture (%) Volatile matter (%) Fixed carbon (%) Ash (%) Pellet density (kg m3) HHV (MJ kg1) Energy density (GJ m3)
CFP 12.59 71.59 14.67 1.15 863 ± 21 18.96 16.36
CFSP 12.61 54.30 18.25 14.84 1160 ± 5 17.54 20.35
CP 12.57 73.56 12.03 1.84 883 ± 12 18.87 16.66
CSP 12.27 55.88 16.70 15.15 1144 ± 7 17.50 20.02
RSP 11.17 63.49 11.02 14.31 1027 ± 7 15.04 15.45
RSSP 12.23 51.26 15.10 21.41 1217 ± 11 15.32 18.64
514 L. Jiang et al. / Energy Conversion and Management 126 (2016) 509–515
Fig. 6. DTA curves of raw biomass pellets and sludge mixed pellets.
4. Conclusions
Table 4
The characteristic combustion parameters of raw biomass pellets and their corresponding sludge mixed pellets.
Pellet sample Ignition temperature Final combustion temperature Temperature at maximum weight loss rate Maximum weight loss rate Residue
(°C) (°C) (°C) (% s1) (%)
CFP 310 531 351 0.69 1.06
CFSP 298 660 492 0.28 15.53
CP 295 569 343 1.29 1.26
CSP 249 530 476 0.37 13.22
RSP 255 469 303 1.61 11.93
RSSP 276 702 301 0.27 21.20
L. Jiang et al. / Energy Conversion and Management 126 (2016) 509–515 515
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