Waste Management xxx (2017) xxx–xxx

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Waste Management
journal homepage: www.elsevier.com/locate/wasman

Combustion characteristics of biodried sewage sludge

Zongdi Hao a, Benqin Yang b, Deokjin Jahng a,⇑
a
Department of Environmental Engineering & Energy, Myongji University, 116 Myongjiro, Cheoingu, Yonginshi, Gyeonggido 17058, Republic of Korea
b
Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, Yunnan 650500, People’s Republic of China

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

Article history: In this study, effects of biodrying on the characteristics of sewage sludge and the subsequent combustion
Received 20 July 2017 behavior were investigated. 7-Day of biodrying removed 49.78% of water and 23.17% of VS initially con-
Revised 25 October 2017 tained in the sewage sludge and increased lower heating value (LHV) by 37.87%. Meanwhile, mass con-
Accepted 3 November 2017
tents of C and N decreased from 36.25% and 6.12% to 32.06% and 4.82%, respectively. Surface of the
Available online xxxx
biodried sewage sludge (BDSS) appeared granulated and multi-porous, which was thought to facilitate
air transfer during combustion. According to thermogravimetric (TG) analysis coupled with mass spec-
Keywords:
trometer (MS) with a heating rate of 10 °C/min from 35 °C to 1000 °C, thermally-dried sewage sludge
Biodrying
Combustion kinetics
(TDSS) and BDSS lost 74.39% and 67.04% of the initial mass, respectively. In addition, combustibility index
Isothermal combustion (S) of BDSS (8.67
108 min2 K3) was higher than TDSS. TG-MS analyses also showed that less nitroge-
Nitrogenous gases nous gases were generated from BDSS than TDSS. It was again showed that the average CO and NO con-
Sewage sludge centrations in exit gas from isothermal combustion of BDSS were lower than those from TDSS, especially
at low temperatures (800 °C). Based on these results, it was concluded that biodrying of sewage sludge
was an energy-efficient water-removal method with less emission of air pollutants when BDSS was
combusted.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction digestate have limited the spreading of anaerobic digestion (Ma

Sewage sludge is an unavoidable byproduct of wastewater
treatment processes that must be properly managed (Folgueras
et al., 2013). Over the past decades, production of sewage sludge
has increased all over the world due to the rapid expansion of
urban cities and wastewater treatment capacities (Magdziarz and
Wilk, 2013b). As one of disposal methods for sewage sludge, land-
filling has been practiced in many regions but brings substantial
risks of soil and groundwater contamination, production of lea-
chate, and land shortages (Werther and Ogada, 1999). Sewage
sludge has also been used as an organic fertilizer and a soil amend-
ment. However, it must be taken into account that sludge may con-
tain hazardous pollutants and microbial pathogens which can
potentially threaten human health and natural environments
(Winkler et al., 2013). Anaerobic digestion, which can reduce the
sewage sludge mass and recover the biogas, is widely practiced
particularly in Europe and Japan. However, long digestion period
is needed because anaerobic microorganisms are slow to be fully
effective (Mata-Alvarez et al., 2000). Moreover, high capital and
operational costs as well as the necessity of further treatment for
⇑ Corresponding author.
E-mail address: djahng@mju.ac.kr (D. Jahng).
et al., 2016).
In many countries, due to the limitation of land resource and
increase of energy demand, incineration has drawn much attention
as an effective approach for reducing the quantity and toxicity of
sewage sludge along with recovering energy (Ma et al., 2016).
Utilization of dried sludge as a solid fuel may provide several ben-
efits that are not found in other treatment alternatives. First of all,
incineration reduces sludge volume because stabilized ash
accounts for 10% or less of the volume of sludge that is mechani-
cally dewatered at wastewater treatment plants (WWTP)
(Folgueras et al., 2003). Moreover, ash from sewage sludge com-
bustion can be used for brick manufacture, agricultural remedia-
tion, and adsorbent preparation (Donatello and Cheeseman,
2013). Secondly, the calorific value of dried sewage sludge
(10,400 kJ/kg) is close to that of brown coal (11,900 kJ/kg)
(Winkler et al., 2013). Therefore, dried sewage sludge can be used
as a renewable fuel replacing fossil fuels (Li et al., 2015). Finally,
compared to the hard coal, high volatile solids (VS) content of sew-
age sludge leads to fast ignition at low temperature in the co-
combustion processes of coal and sludge (Magdziarz and Wilk,
2013b; Otero et al., 2002).
Although sewage sludge is usually mechanically dewatered at
WWTP, moisture content (MC) is still as high as 80–85 wt% in
the dewatered sludge (Cai et al., 2016). When considering combus-

https://doi.org/10.1016/j.wasman.2017.11.008
0956-053X/Ó 2017 Elsevier Ltd. All rights reserved.

Please cite this article in press as: Hao, Z., et al. Combustion characteristics of biodried sewage sludge. Waste Management (2017), https://doi.org/10.1016/
j.wasman.2017.11.008
2 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx

Nomenclature

Acronyms LHV lower heating value (kJ/kg)

BDSS biodried sewage sludge MC moisture content (wt%)
BVS biodegradable volatile solids TDSS thermally-dried sewage sludge
DSC differential scanning calorimetry (W/g) TG-MS thermogravimetric coupled with mass spectrometer
DTG Derivative thermogravimetry (%/ min) TS total solids (wt%)
HHV higher heating value (kJ/kg) VS volatile solids (wt%)

tion as a final disposal option, moisture contained in sludge needs diameter) was prepared by spreading the dewatered sludge and
to be removed because direct incineration of wet sludge is not air-dried for a couple of weeks until the MC became constant
cost-efficient and may create unstable burning (Ma et al., 2016). (Yang et al., 2014). For preparing the drying feedstock, dewatered
Obviously, conventional thermal drying methods can be used to sludge and air-dried sludge were thoroughly mixed manually at
remove moisture from sludge, but these processes consume much the mixing ratio of 3:1 (w/w, wet basis) for at least 30 min. The
energy due to high latent heat of water evaporation and structural characteristics of the raw materials are presented in Table 1.
features of sewage sludge. For example, loosely-packed extracellu-
lar polymeric substances (EPS) in the sludge contain a high content 2.2. Biodrying
of sticky matters, which lowers the sludge dewaterability (Cai
et al., 2016). For lab-scale biodrying, an air-tight 28.3 L cylindrical vessel
In contrast, biodrying is regarded as an energy-saving method (inner diameter of 300 mm, height of 450 mm) made of PMMA
because water is removed from waste materials by using the meta- (polymethyl methacrylate) which was described elsewhere (Yang
bolic heat produced from aerobic microbial degradation of et al., 2013). 10 kg of the feedstock was filled into the biodrying
biodegradable VS (BVS) contained in the waste itself (Yang et al., reactor and the air flow rate was kept at 2.5 L/min [0.045 m3/hkg
2014). Recently, the changes in micro-structure and EPS of sludge TS (total solids)]. During biodrying, turning and mixing of the reac-
and the mechanism of free water release during biodrying were tor content were not carried out until the sludge temperature
also studied (Cai et al., 2016). The sticky components in sludge returned to ambient temperature for minimizing heat loss and
were decomposed during biodrying, and irregular pore channels maximizing water evaporation. After biodrying, the biodried pro-
in the sludge particles were formed (Han et al., 2012). Meanwhile, duct was completely removed from the reactor and weighed. The
bound water in sludge flocs was released during high temperature matrix was then mixed thoroughly for at least 30 min by hand
period which was induced by BVS degradation (Cai et al., 2016). for measuring MC and VS. For the biogenic fraction, calorific value,
Most studies on combustion has been focused on coal and elemental composition determination, TG-MS analysis and
(Folgueras et al., 2003), thermally-dried sewage sludge (TDSS) isothermal combustion experiments, the biodried product was fur-
(Magdziarz and Wilk, 2013b), and municipal solid waste (MSW) ther dried in a dry oven (SOF-W 105, SciLab, Korea) at 105 °C for
(Liu et al., 2016). In many studies, thermogravimetry (TG) was used 24 h, and termed as BDSS. At the same time, TDSS was prepared
to investigate combustion and/or co-combustion behaviors of var- by thermally drying the feedstock in a dry oven at 105 °C for 24
ious fuels at different heating rates (Li et al., 2009; Otero et al., h without prior biodrying.
2007). Gaseous emissions from combustion of fuels were also ana-
lyzed by using TG connected with mass spectrometry (MS) to
obtain relative real-time yields of various emission gases (Wang 2.3. TG-MS analysis
et al., 2016). In addition, isothermal combustion characteristics
and gaseous pollutant emission of TDSS and MSW were also For TG-MS analysis, BDSS and TDSS were pulverized with a
reported in recent years (Shao et al., 2013; Tang et al., 2012). grinder (HR2084, Xin Sheng Electrical Co., China) and then passed
Although many studies have revealed that biodrying affects the through a 63 lm sieve. A thermal analysis system (SDT Q600, TA
contents of organic matter (Yang et al., 2014), chemical composi- instruments, Delaware, USA) was used to simultaneously register
tions (Zhao et al., 2011), and calorific values (Tambone et al., TG signals with an accuracy of 103 mg and differential scanning
2011) of the solid wastes, to the best of our knowledge, neither fuel calorimetric (DSC) signals, by which both mass loss and heat flow
characteristics of biodried sewage sludge (BDSS) nor its combus- profiles were obtained during combustion. TG and DSC signals
tion behaviors has been extensively studied.
In this study, dewatered sludge mixed with air-dried sludge as a Table 1
bulking agent was biodried and subsequently thermally dried (ter- The characteristics of the raw materials.
med as BDSS). For comparison, TDSS was also prepared by ther-
Dewatered sludge Air-dried sludge
mally drying the sludge mixture at 105 °C for 24 h without (bulking agent)
biodrying step. The heating values, combustion characteristics,
MC (wet basis, wt%) 85.94 ± 0.08 14.40 ± 0.25
compositions of gaseous products, and isothermal combustion VS/TS (dry basis, wt%) 75.41 ± 0.07 74.60 ± 0.18
characteristics of these two dried sludge were analyzed and com- Bulk density (g/cm3) 1.04 ± 0.62 0.52 ± 0.01
pared. It was expected that these results could provide valuable HHVa (kJ/kg) 16,956 ± 171 16,209 ± 194
information on combustion of BDSS. LHVb (kJ/kg) 283 ± 24 13,521 ± 46
Elemental composition (dry basis, wt%)
C 38.55 36.14
2. Materials and methods H 5.85 5.42
O 24.65 26.67
2.1. Raw materials N 6.01 6.15
S 1 1.05

The dewatered sludge was obtained from a belt press facility at a

HHV: Higher heating value.
b
a WWTP in Yongin, Korea. The air-dried sludge (0.05–4.5 mm in LHV: Lower heating value.

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 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx
were logged every 0.5 s. At the same time, gaseous emissions were
analyzed by using a mass spectrometer (TA Discovery, TA instru-
ments, Delaware, USA) coupled to the TG. 15 mg of BDSS and TDSS
were loaded onto the system and heated from 35 °C to 1000 °C at
the heating rate of 10 °C/min in the presence of pure oxygen flow-
ing at 50 mL/min. The evolved gaseous products includingNH3/OH,
HCN, CO, NO, HNCO, CO2 and NO2 were monitored. Relative yields
of nitrogenous gases were determined by integrating ion current
intensities (nA) with respect to time, and then the integrals were
normalized by using integrated NH3/OH current intensity of TDSS
as a fiducial value (Wang et al., 2016).
2.4. Isothermal combustion simulation
In order to better understand gaseous emission characteristics
of TDSS and BDSS, isothermal combustion experiments were con-
ducted in a horizontal tube furnace (FT-860, Daihan Scientific,
Korea) connected to a gas analyzer (Multi-Master, Sensoronic Co.,
Korea) as shown in Fig. 1. Before combustion experiments, the
gas analyzer was zeroed using the ambient air as a zeroing gas.
The compressed air was fed at the flow rate of 2 L/min and the
combustion temperature was set at 600, 700, 800, 900 and 1000
°C. When the temperature of the furnace reached the set point,
an alumina boat with 0.1 ± 0.001 g of a pulverized sludge sample
was loaded into the furnace, which was then quickly sealed with
an insulating plug. The gas analyzer was connected to the furnace
and started to receive the exit gas to measure the concentrations of
CO, NO, SO2, CO2 and O2 in the exit gas. The retention time of
sludge in the furnace was 10 min, during which time-course data
were recorded online every second. The detection ranges of CO,
NO, SO2, CO2 and O2 were 0–3000 ppmv, 0–5000 ppmv, 0–2000
ppmv, 0–25% (v/v) and 0–21% (v/v), respectively, with precision
ranges of ±10 ppmv, ±3 ppmv, ±1 ppmv, ±0.01% and ±0.05%,
respectively.
2.5. Sampling and analytical methods
The MC and VS were measured according to the Standard Meth-
ods (APHA, 2005). To determine the content of biogenic organic
fraction, which was defined as the material produced in natural
processes by living organisms but not fossilized or derived from
fossil resources, 0.2 g of dried sludge were added into 30 mL of
13.50 M H2SO4 for 16 ± 2 h and then 6 mL of 1.55 M H2O2 were
added for 5 ± 1 h. The digested samples were filtered over a pre-
weighed Whatman glass microfiber filter (Little Chalfont, UK) with
a pore size of 1.2 lm. The residue together with the filter was dried
at 105 °C for 24 h and then combusted at 550 °C for 30 min. The
biogenic fraction (vB) was calculated by Eq. (1):


mresidue  mresidue  ash
vB ¼ 1  þ ash
100%
msample
Fig. 1. The schematic diagram of the isothermal combustion system. 1, Compressed air; 2, air flow meter; 3, tube furnace; 4, temperature sensor; 5, alumina boat with sludge
sample; 6, temperature controller; 7, insulating plug; 8, gas analyzer; 9, exit gas.
Please cite this article in press as: Hao, Z., et al. Combustion characteristics of biodried sewage sludge. Waste Management (2017), https://doi.org/10.1016/
j.wasman.2017.11.008
3
where ash was the ash content of the sample (dry basis, wt%)
mresidue and mresidue-ash were the weights (g) of residue together
with the filter after drying at 105 °C and combustion at 550 °C,
respectively, and msample was the weight (g) of dried sludge sample
(Tambone et al., 2011). The higher heating values (HHV) were mea-
sured using an oxygen bomb calorimeter (Parr 6400, Parr Instru-
ment Co., Illinois, USA), and lower heating values (LHV) was
calculated according to He (2011). Bulk density was measured by
weighing the mass of sludge with known volume (Zhao et al.,
2010). Elemental compositions of C, N, H, S and O were analyzed
using an elemental analyzer (Flash EA1112, Thermo Finnigan-CE
Instruments, Italy). Micro-structures of the samples were observed
by using a scanning electron microscope (SEM) (S-4800, Hitachi,
Japan) at an accelerating voltage of 20 kV (Han et al., 2012).
2.6. Kinetic calculations
As a comprehensive index characterizing the combustion pro-
cess, combustibility index, S (Li et al., 2014; Liu et al., 2016), was
calculated as:
ðdw=dtÞmax ðdw=dtÞmean
S¼ ð2Þ
T2i T0
where ðdw=dtÞmax and ðdw=dtÞmean were the maximum and average
mass loss rate, i.e., maximum and average derivative thermo-
gravimetry (DTG,%/min) during heating process of TG analysis. Ti
was the ignition temperature (K) obtained by the TG-DTG tangent
method (Li et al., 2009). T0 was the burnout temperature (K) at
which the DTG profile reached 1%/min combustion rate at the tail
end of the curves (Chen et al., 2015).
In addition, the modified Arrhenius equation was adopted to
describe the temperature dependence of the heterogeneous solid
state reactions (Liu et al., 2016):


da E
¼ A exp  fðaÞ ð3Þ
dt RT
in which a was the conversion rate (dimensionless), t was time
(min), T was the combustion temperature (K) at time t, E was the
activation energy (kJ/mol), R was the universal gas constant
(8.314 J/molK) and A was the pre-exponential factor (min1).
The f (a) was the reaction model function generally described as
f(a) = (1  a)n, where n was the reaction order. The conversion rate
a was expressed as:
m0  mt
a¼ ð4Þ
m0  m1
where m0 was the initial mass of the sample (mg), mt was the mass
ð1Þ of sample at time t (mg), and m1 was the final mass of the sample
in the reaction (mg).
4 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx

In non-isothermal TG conditions, by dividing with constant organic constituents of wastewater (Winkler et al., 2013). The non-
temperature increase rate b (b = dT/dt), the Eq. (3) was modified biogenic fraction with a proportion around 10% of VS was thought
to the following expression: to be plastics or synthetic polymers in the sewage (Tambone et al.,

 2011). 49.78% of water and 23.17% of VS initially contained in the
da A E
¼ exp  fðaÞ ð5Þ feedstock were removed during 7 days of biodrying. It was thought
dT b RT
that air-dried sludge supplemented BVS as well as abundant
where b was the heating rate (K/min) during TG analysis. After inte- microorganisms for biodrying so that a large amount of heat was
gration of the Eq. (5), the following equations were obtained: evolved in a short time, allowing the fast evaporation of water
  
 from the feedstock (Zhao et al., 2011). It was also suspected that
lnð1  aÞ AR 2RT E
ln ¼ ln 1   ðn ¼ 1Þ ð6:1Þ porous structure of air-dried sludge provided efficient air transport
T 2 bE E RT throughout the biodrying matrix (Yang et al., 2014).
" # 
 In addition, mass of biogenic fraction decreased by 0.53 kg,
1  ð1  aÞ1n AR 2RT E which accounted for almost 93% of the VS loss. As VS/TS decreased
ln ¼ ln 1  ðn – 1Þ ð6:2Þ
2
T ð1  nÞ bE E RT from 74.77% to 68.98%, HHV of the mixture decreased by 11.12%
after biodrying (Zhao et al., 2010). However, it should be noticed
A straight line with the highest correlation index (R2) of ln[(ln that the LHV increased by 37.87% after biodrying compared to
(1  a))/T2] versus 1/T (n = 1) or ln[(1  (1  a)1n)/(T2(1  n))] the feedstock as MC decreased from 67.10% to 55.15%. The final
versus 1/T (n – 1) was obtained by calculating an optimal reaction LHV of the biodried product was as high as 5,355.86 kJ/kg, which
order (n) using the Visual Basic for Applications (VBA) in Excel was known to be sufficient for self-sustaining combustion (Zhu
2013. The kinetic parameters, activation energy E, and pre- et al., 2013). These results indicated that biodrying could be an
exponential factor A were calculated by using the slope and the energy-saving and efficient pretreatment method for removing
intercept values of the straight lines (Folgueras et al., 2003). moisture and thus enhancing LHV of the wet wastes (Tambone
et al., 2011). In Table 2, VS and ash contents, HHV, biogenic and
3. Results and discussion non-biogenic fractions, and elemental compositions were deter-
mined based on dry basis. In other words, thermally-dried samples
3.1. Biodrying of the mixture of dewatered and air-dried sludge were used for measuring those parameters. Since BDSS was pre-
pared by thermally drying (105 °C, 24 h) the biodried product,
As shown in Table 1, two raw materials, dewatered sludge and and TDSS was prepared by thermally drying the fresh mixture
air-dried sludge, showed similar characteristics in terms of VS con- without biodrying, above-mentioned parameters in Table 2 could
tent, HHV and elemental composition. Since air-dried sludge con- be interpreted as the differences between TDSS and BDSS. As VS
tained less moisture, its LHV was much higher than that of was consumed during biodrying, the mass contents of C and N
dewatered sludge. The air flow rate of biodrying was 0.045 m3/h decreased from 36.25% and 6.12–32.06% and 4.82%, respectively
kg TS, which was in the middle of the previously optimized ranges (Table 2). According to the respiration reactions proposed by
(0.035–0.06 m3/h kg TS) (Ma et al., 2016; Yang et al., 2014; Zhao Yang et al. (2013) and Zhao et al. (2010), organic carbon in the
et al., 2010). The MC of the mixture was 67.10 wt% (Table 2), which sludge was consumed by the microorganisms for energy produc-
has known to be in the optimal MC range for biodrying (Huiliñir tion, and CO2 was emitted in the exit gas. Nitrogen in sewage
and Villegas, 2015; Yang et al., 2014). This mixture was identically sludge is known to be mainly converted to and released as NH3,
used for preparing BDSS and TDSS. In the mixture, biogenic fraction which can be easily recovered as ammonium sulfate from the exit
accounted for almost 90% of VS. In fact, the VS of sludge is a mix- gas in an acidic gas scrubber (Winkler et al., 2013).
ture of excess biomass generated in the biological digestion of the
3.2. Morphology and surface structures of BDSS and TDSS
Table 2
Characteristics of the sludge mixture before and after biodrying.
Fig. 2 shows the macroscopic and microscopic surface struc-
Before After Changea tures of TDSS and BDSS. TDSS, the mixture of dewatered and air-
biodrying biodrying (%) dried sludge thermally-dried at 105 °C for 24 h, appeared as large
Total weight (kg) 10.0 6.1 38.90 agglomerated particles, while particles of BDSS that were biodried
Volume (dm3) 16.3 10.6 34.97 first and then thermally-dried were finer and smaller. This smaller
Density (g/cm3) 0.62 0.57
particle size of biodried sludge was thought to be resulted from
Water (kg) 6.71 3.37 49.78
MC (Wet basis, wt%) 67.10 ± 1.51 55.15 ± 1.36 biological degradation of sticky and viscous components of sewage
TS (kg) 3.29 2.74 16.72 sludge such as polysaccharide, protein and lipids. Cai et al. (2016)
VS (kg) 2.46 1.89 23.17 also observed that degradation of EPS in sludge caused demolished
VS/TS (Dry basis, wt%) 74.77 ± 0.45 68.98 ± 1.39 floc structures. It was also suspected that the microbial decompo-
Ash (kg) 0.86 0.85 1.16
Biogenic fraction (kg) 2.19 1.66 24.20
sition of large molecular components during biodrying resulted in
Biogenic fraction (g/kg TS) 665.29 ± 1.47 601.27 ± 4.85 a granulated and multi-porous micro-structures of biodried prod-
Non-biogenic fraction (kg) 0.27 0.23 14.81 ucts as Han et al. (2012) suggested. For example, degradation of
Non-biogenic fraction 84.13 ± 1.47 81.80 ± 4.85 EPS in sludge caused demolished floc structures (Cai et al., 2016).
(g/kg TS)
On the contrary, surface of TDSS appeared compact and viscous
HHV (kJ/kg) 16,380 ± 182 14,557 ± 44 11.12
LHV (kJ/kg) 3885 ± 61 5356 ± 20 +37.87 because thermal drying of highly-wet sludge created shrunken
3884.82 ± 60.78 5355.86 ± 19.92 and angular structure (Fig. 2). Scaly and multi-porous structure
Elemental composition (wt.%, dry basis) of BDSS was expected to facilitate air and heat transfer during com-
C 36.25 32.06 bustion or pyrolysis processes (Han et al., 2012).
H 5.56 5.18
O 26.52 25.17 3.3. TG analysis of TDSS and BDSS
N 6.12 4.82
S 1.03 1.17
Sewage sludge combustion is a complicated process in which
a
Change = [(After-Before)/Before] * 100%. drying, devolatilization, heterogeneous reaction, ignition and burn-

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 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx 5

Fig. 2. Macro- and micro-structures of TDSS (left) and BDSS (right).

ing occur (Magdziarz and Wilk, 2013b). In TG analysis with a heat-
ing rate of 10 °C/min from 35 °C to 1000 °C, TDSS and BDSS lost
74.39% and 67.04% of the initial mass, respectively (Fig. 3A). The
weight loss of BDSS was lower than that of TDSS because of the
lower VS content (Table 2). As shown in Fig. 3B and Table 3, the
ignition temperature (Ti) of BDSS (229.9 °C) was slightly higher
than that of TDSS (223.8 °C), and this might be due to that the
flammable VS was also easily biodegradable and was consumed
during biodrying. Similarly to Ti, the temperature of maximum
mass loss rate (Tp) of BDSS (279.3 °C) was also slightly higher than
that of TDSS (275.4 °C). On the contrary, the burnout temperature
(T0) of BDSS (470.3 °C) was lower than that of TDSS (484.1 °C).
Since the readily biodgradable VS was consumed during biodrying,
as a result, less char would be formed and thus the burnout of the
combustible components occurred at a lower temperature for
BDSS. Ti and T0 of coal are known to be 352–442 °C and 725–
970 °C (Li et al., 2009; Otero et al., 2011), respectively, hence,
sludge could be ignited and also burnt out at lower temperatures
because of easily decomposable components such as bacterial cells.
Therefore it was expected to be easy to initiate combustion of the
mixture of sewage sludge and coal (Otero et al., 2007).
As shown by DTG curves in Fig. 3B, the main combustion of
TDSS and BDSS occurred between 200 to 580 °C for both TDSS
and BDSS. When the temperature was higher than 600 °C mass loss
was brought to an end by thermal decomposition (Fig. 3A). In TDSS
combustion, the first DTG peak located between 200 °C to 365 °C

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6 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx
Fig. 3. (A) TG, (B) DTG and (C) DSC curves obtained from non-isothermal
combustion of TDSS and BDSS.
indicated that about 49.92% of the initial mass was lost during this
range of combustion temperature. This mass loss was thought to
be resulted from the devolatilization of sludge (Magdziarz and
Wilk, 2013b). The second DTG peak representing char oxidation
(Li et al., 2014) appeared from 365 °C to about 580 °C, with a
weight loss contribution of about 23.28%. In the case of BDSS, the
first peak with a mass loss of 47.09% appeared in the interval from
200 °C to about 365 °C, which was similar to that of TDSS. How-
ever, the weight loss in the second interval from 365 °C to about
580 °C was as low as 17.73%, which was obviously lower than that
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of TDSS. It was suspected that, most of volatile solids in sludge
sample was devolatilized while the char and/or fixed solids were
not yet oxidized. Thus, a lower weight loss rate was observed,
resulting in the valleys on the DTG curves between 300 to 400
°C. For comparing combustion characteristics of TDSS and BDSS,
results in Fig. 3 were analyzed and summarized in Table 3. The
maximum weight loss rates were 6.27 and 7.73%/min at 275.4 °C
and 279.3 °C for TDSS and BDSS (Fig. 3B and Table 3), respectively.
These results indicated that the volatile release upon combustion
of BDSS was more evident than TDSS in the first stage. It is well
known that the sludge is complex in chemical composition
(Magdziarz and Wilk, 2013b), and the differences in combustion
behavior of the BDSS and TDSS were mainly caused by aerobic
digestion during biodrying. Barneto et al. (2009) found that aerobic
digestion of sludge during composting reduced the hemicellulosic
and cellulosic fractions while seldom affected non-biodegradable
matters composed of lignin-plastic fraction. During biodrying, sol-
uble fractions were the main substrates for microorganisms, which
contributed to the initial temperature rise (Zhao et al., 2011). Then,
in the thermophilic phase, organic fractions and free water release
occurred (Cai et al., 2016). The differences in combustion behavior
between TDSS and BDSS indicated that biodrying changed the
organic composition and its content in the sludge.
According to DSC results (Fig. 3C and Table 3), heat release from
combustion of both TDSS and BDSS started at 200 °C and formed
two peaks as expected from the DTG curves (Fig. 3B). The first
exothermic peak values of TDSS and BDSS were 15.2 W/g at
312.2 °C and 15.7 W/g at 301.5 °C, respectively. The second
exothermic peak of TDSS with 14.7 W/g appeared at 434.5 °C while
that of BDSS was only 8.8 W/g at 405.4 °C (Table 3). The DSC and
DTG curves matched very well in one-to-one manner for both TDSS
and BDSS. It was also observed that the main differences between
TDSS and BDSS were the exothermic characteristics and peak val-
ues of the second stage, which of TDSS were higher than those of
BDSS (Fig. 3C). Similarly to DTG curves (Fig. 3B), valleys were
observed on DSC curves due to the low weight loss rates between
300 to 400 °C. From the DSC curve, total heat productions in the
first peaks were about 8055 J/g and 7696 J/g for TDSS and BDSS,
respectively. However, in the second stage, the heat production
was 8381 J/g for TDSS while BDSS produced only 5455 J/g. From
these results, it was speculated that the lower HHV of BDSS
(Table 2) was due to the lower heat production in the second stage.
The differences observed in DTG curves in the second stage might
be related with combustion of the char previously formed from the
VS (Barneto et al., 2009). Without biodrying, most BVS in the TDSS
were conserved, and, as a result, more char contributed more heat
production in the second exothermic stage.
Biodrying enhanced the combustion rate of sewage sludge
because the weight loss rate was higher than that of TDSS (Table 3
and Fig. 3B). The combustibility index, S, is a comprehensive
parameter characterizing the combustion process, and higher S is
known to indicate better combustion performances of solid fuels
(Liu et al., 2016). As shown in Table 3, the S of BDSS was as high
as 8.67
108 min2 K3 and was much higher than that of the
TDSS because of the higher maximum weight loss rate and lower
T0 of BDSS. However, the VS content and calorific values of the
BDSS decreased due to the VS consumption of the sludge by
biodrying. To overcome this problem, co-combustion of BDSS with
coal or other biomass might be a good strategy (Li et al., 2014;
Otero et al., 2002). Nevertheless, BDSS showed higher S and lower
T0, which would facilitate its combustion (Liu et al., 2016).
3.4. Combustion kinetics
In order to investigate effects of biodrying on combustion kinet-
ics of the sludge, the modified Arrhenius equation was adopted to
 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx 7

Table 3
Non-isothermal combustion characteristics of TDSS and BDSS.

Material Ti (°C)a (dw/dt)max Tp (°C)b T0 (°C)c (dw/dt)mean S/108 Temperature DSCmax Tme (°C) n E (kJ/mol) ln A (min1) R2
(%/min) (%/min) (min2K3)d range (W/g)
TDSS 223.8 6.27 275.4 484.1 2.07 6.94 200–365 °C 15.2 312.2 1.62 101.7 20.67 0.9619
365–500 °C 14.7 434.5 1.68 176.9 29.60 0.9407
BDSS 229.9 7.73 279.3 470.3 2.11 8.67 200–365 °C 15.7 301.5 1.66 105.3 21.46 0.9661
365–500 °C 8.8 405.4 1.77 175.4 29.65 0.9326
a
Ti: ignition temperature obtained by the TG-DTG tangent method.
b
Tp: temperature at the maximum mass loss rate.
c
T0: burnout temperature at which the DTG profile reached 1%/min at the tail end of the curves.
d
S: combustibility index calculated by Eq. (2)
e
Tm: temperature of maximum energy release during non-isothermal combustion.

describe the temperature-dependent TG process. The activation

energy E and pre-exponential factor A were calculated and sum-
marized in Table 3. High linear correlation indices (R2) indicated
that the reaction model fitted the experimental data very well.
The activation energy is considered as the energy threshold that
must be overcome to start combustion (Otero et al., 2011). The
activation energy of BDSS at the first stage was slightly higher than
that of TDSS, which meant that biodrying caused the threshold to
slightly increase when combustion started. At the second stage,
the BDSS showed a lower activation energy than TDSS. For
temperature-dependent reaction, the pre-exponential factor is
usually positively correlated with the reactivity (Folgueras et al.,
2013). Compared to TDSS, the slightly higher lnA of BDSS at two
stages implied that combustion of BDSS was more facile. Neverthe-
less, there was no obvious differences between TDSS and BDSS for
both pre-exponential factor and activation energy. These results
demonstrated that biodrying did not exert negative influences on
the combustion of the sludge. Rather, biodrying provided higher
reactivity for combustion although a part of BVS was consumed
by microbial degradation.

3.5. MS analysis

3.5.1. Nitrogenous gases release

Since nitrogen content of the sludge was reduced by biodrying
(Table 2), it was anticipated that the nitrogenous composition of
emission gas from combustion of BDSS might be different from
that of TDSS. In order to monitor nitrogenous gas evolution from
the sludge combustion, exit gas from TG was analyzed by using
MS. As shown in Fig. 4, most nitrogenous gases were emitted in
the temperature range between 200 and 600 °C, which indicated
that most nitrogenous substances contained in sewage sludge
were readily volatile. In case of TDSS, two peaks appeared in this
temperature range of the TG heating process. In case of BDSS,
two major peaks were observed for HCN and NO, similarly to TDSS.
However, there appeared only one major peak for NH3, HOCN and
NO2 in the low temperature range (200–400 °C). The valleys
between the peaks were speculated to be due to the low weight
Fig. 4. Nitrogenous gas evolution profiles of TDSS and BDSS.
loss rate observed in DTG curves (Fig. 3B). For both TDSS and BDSS,
the NH3 ion current intensity was stronger than other nitrogenous
gases because the signal might be contributed not only by NH3 but rocyclic compounds were decomposed to HCN and further oxi-
also by OH (Wang, et al., 2016). It was also observed that the NH3 dized to NOx (Becidan et al., 2007). In short, as Wang et al.
showed a narrow release profile with a peak appeared at 280 °C (2016) pointed out, nitrogen in sewage sludge was converted to
and was emitted little when the temperature was higher than HCN, NH3 and other nitrogenous volatile species or intermediates
400 °C (Fig. 4). Nitrogen is mainly from proteins, amino acids, for subsequent reactions in the low-temperature region. NOx is
lower amines and various nitrogen-containing heterocyclic com- one of groups of chemical species that can harm the environment
pounds (e.g., pyrroles, pyridines, etc.) in sewage sludge (Wang and human health by forming photochemical smog (Otero et al.,
et al., 2016; Werther and Ogada, 1999). It was reported that 2002) and corroding metallic materials (Magdziarz and Wilk,
protein-N was converted into amine-N first and transferred to 2013a). As shown in Table 4, it was found in this study that total
heterocyclic compounds (e.g., diketopiperazine, nitriles) with the relative yield of the nitrogenous gases from BDSS was 1.49,
release of NH3 during the heating process in TG (Wang et al., whereas that of TDSS was 1.86. Li et al. (2014) reported that, dried
2016). When the temperature continued to rise, the residual hete- sewage sludge emitted less nitrogenous gases during combustion

Please cite this article in press as: Hao, Z., et al. Combustion characteristics of biodried sewage sludge. Waste Management (2017), https://doi.org/10.1016/
j.wasman.2017.11.008
8 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx
Table 4
Relative yields of nitrogenous gases from TDSS and BDSS.
Material NH3 HCN HNCO NO NO2 Total
TDSS 1.00 0.28 0.22 0.33 0.03 1.86
BDSS 0.76 0.22 0.19 0.30 0.02 1.49
than wheat straw, corn stalks and cotton stalks. Biodrying reduced
the nitrogen content even further, which led to less nitrogenous
gas emission during combustion. Therefore, BDSS was expected
to be an environment-friendly renewable fuel.
3.5.2. CO2 and CO release
During TG-MS analysis, CO2 and CO were released in the form of
two peaks similarly to nitrogenous gases (Fig. 5). It has been
reported that the CO2 emission is mainly from devolatilization as
well as combustion of organic fraction and char (Folgueras et al.,
2013; Magdziarz and Wilk, 2013b). The first peak of CO2 in the
volatile burning phase (200–400 °C) was larger than the second
peak in the char oxidation phase (400–600 °C). It needs to be
noticed that the second CO2 emission peak of BDSS was slightly
smaller than that of TDSS because carbon content decreased after
biodrying (Table 2).
As show in Fig. 5, CO production was lower for BDSS than TDSS
during the entire heating process of TG. Compared to TDSS, lower
CO emission indicated by lower ion current (m/z = 28) from BDSS
combustion could be attributed to the following factors. Firstly, C
content decreased from 36.25% to 32.06% because of the BVS
biodegradation during biodrying process (Table 2). Secondly, per-
haps more importantly, biodrying produced porous and loose
structure as VS and water were removed (Fig. 2). This multi-
porous structure of BDSS was thought to enhance mass and heat
transfers during the heating process of TG, reduced incomplete
combustion, and thus suppressed the CO formation.
3.6. Pollution characteristics of isothermal combustion
3.6.1. CO emission
In order to compare gas emission during a real combustion pro-
cess, TDSS and BDSS were isothermally combusted at 600–1000 °C
Fig. 5. CO2 and CO evolution profiles of TDSS and BDSS obtained from TG-MS
analysis.
Please cite this article in press as: Hao, Z., et al. Combustion characteristics of biodried sewage sludge. Waste Management (2017), https://doi.org/10.1016/
j.wasman.2017.11.008
in a tube furnace and emitted concentrations of CO, NO, and SO2
were analyzed. As shown in Fig. 6A, there appeared two CO peaks
emitted at 20–100 s and 100–380 s during the isothermal combus-
tion at 600 °C. The highest CO concentrations in the first peaks
from combustion of TDSS and BDSS were 420 ppmv and 285 ppmv,
respectively. The second peaks of CO reached 891 ppmv and 832
ppmv for TDSS and BDSS, respectively. During the initial 100 s, it
was thought that highly volatile fractions contained in the sludge
were thermally decomposed and then CO2, CO as well as char were
produced (Shao et al., 2013). Subsequently, the second CO peaks,
which lasted until 380 s, were formed due to the incomplete com-
bustion of the fixed carbon in the char (Jin et al., 2016). The gaps
between the sludge devolatilization and char oxidation resulted
in the valleys of CO concentration at 100 s for both TDSS and BDSS.
After 380 s, the CO emission almost ceased because the com-
bustible components were exhausted. Fig. 6D shows average con-
centrations of air pollutants emitted from TDSS and BDSS
combusted at 600–1000 °C. Average CO concentration in the exit
gas from BDSS combustion at 600 °C for 600 s was 219.32 ppmv,
which was 15.68% lower than that of TDSS. Reduced CO emission
implied that complete combustion was promoted in BDSS because
biodrying modified the sludge microstructure to be more porous
(Fig. 2) and thereby the oxygen transfer was facilitated. The aver-
age CO concentrations of BDSS obtained from combustion at higher
temperatures were also lower than those of TDSS. Besides, as com-
bustion temperature increased from 600 °C to 1000 °C, CO concen-
tration in the emission gas decreased sharply. When temperature
increased to 800 °C, CO was not detected both for TDSS and BDSS,
indicating that the CO emission could be eliminated by increasing
combustion temperature.
3.6.2. NO and SO2 emission
NO and SO2 were mainly emitted during 50–300 s when
isothermally combusted at 600 °C (Fig. 6B and C) and other tem-
peratures (data not shown). When combusted at 600 °C, the high-
est NO concentrations were 222 ppmv and 190 ppmv for TDSS and
BDSS, respectively. In this study, NO was measured because it was
reported that NO was the dominant species in the combustion pro-
cess with NO2 and N2O being less than 5% of the total NOx (Shao
et al., 2013; Werther and Ogada, 1999). Fig. 6D shows that the
average NO concentrations were 23.10 ppmv and 16.99 ppmv for
TDSS and BDSS, respectively, when combusted at 600 °C. The aver-
age NO concentration in the emission gas from BDSS combustion
was lower than that of TDSS at various temperatures even though
there was no significant difference at higher temperatures (800
°C). The elemental content of N in sludge decreased from 6.12%
to 4.82% (Table 2) after biodrying, thus the NO emission was also
reduced in BDSS combustion. Average NO concentration increased
slightly up to 800 °C and then decreased for both TDSS and BDSS.
The similar results were also observed by Tang et al. (2012), who
showed that the maximum NO emission temperature was 800 °C
for isothermal combustion of MSW. It was postulated that NO
emission could be influenced by the interaction of many factors
during combustion, for instances, deficiency of O2 in the furnace
(weakly oxidizing atmosphere), heterogeneous reactions between
gas (NO) and solid (char) on the surface of char, and homogeneous
reaction of NO with reducing agents (e.g., CO and NH3) (Shao et al.,
2013). In this study, no NH3 was observed during the isothermal
combustion process since most NH3 was emitted at lower temper-
atures (400 °C) according to the TG-MS data (Fig. 4). Therefore,
CO might be the main reducing agent for NO reduction in the gas
phase (Shao et al., 2013) during isothermal combustion at temper-
atures higher than 600 °C. The increase of NO emission from 600 °C
to 800 °C might be due to the sharp decrease of CO concentration
in this temperature range (Fig. 6D), while the decrease of NO emis-
sion from 800 °C to 1000 °C was attributed to O2 deficiency (data
 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx
Fig. 6. Time-courses of concentrations of (A) CO, (B) NO, and (C) SO2 emitted from isothermal combustion at 600 °C, and (D) average concentrations of air pollutants released
during isothermal combustion at various temperatures.
not shown) and char formation resulted from instantaneous com-
bustion of sludge at high temperatures (Shao et al., 2013). Accord-
ing to the conversion ratio calculation based on Yang et al. (2016),
the conversion ratio of N to NO in this study was only 4.72% and
4.35% for TDSS and BDSS at 600 °C, respectively. It was thought
that low conversion rate was obtained because CO and the residual
char reduced NO (Yang et al., 2016), which might have occurred
immediately upon the formation of NO as shown below (Dong
et al., 2010).
Char
C þ NO ! CO þ 1=2N2
Char
CO þ NO ! CO2 þ 1=2N2
Besides the combustible fraction, sludge also contains various
metallic oxides in the ash fraction, which might catalyze the NO
reduction at high temperature conditions (Li et al., 2014). In case
of this, blending sludge with coal or biomass would supply cata-
lysts for NO reduction and decrease the pollutant emission of the
solid fuel combustion.
The maximum SO2 concentrations were respectively 104 ppmv
and 105 ppmv for TDSS and BDSS (Fig. 6C). Although the S content
in BDSS (1.17 wt%, dry basis) was slightly higher than that of TDSS
(1.03 wt%) (Table 2), average SO2 concentrations in emitted gas
from BDSS combustion was almost the same with TDSS when the
combustion temperature was lower than 800 °C. However, SO2
emission from BDSS combustion was higher than those of TDSS
at temperatures higher than 800 °C (Fig. 6D). As combustion tem-
perature increased, average SO2 concentrations in the emitted gas
also increased, and the concentration differences between TDSS
and BDSS became larger (Fig. 6D). The sulfur conversion ratio,
Please cite this article in press as: Hao, Z., et al. Combustion characteristics of biodried sewage sludge. Waste Management (2017), https://doi.org/10.1016/
j.wasman.2017.11.008
9
which was defined as the S converted to SO2 accounted for the total
S in the sludge sample (Yang et al., 2016), was 51.61% and 46.58%
for TDSS and BDSS at 600 °C. However, when the combustion tem-
perature was 1000 °C, the sulfur conversion ratios of both TDSS and
BDSS were nearly 100%. These results indicated that conversion of
sulfur in sludge to SO2 was more complete as the combustion tem-
perature increased (Shao et al., 2013). The higher SO2 emissions at
higher temperatures have been reported by Tang et al. (2012) who
dealt with MSW and Shao et al. (2013) who studied with TDSS. For
capturing SO2 in exit gas, desulphurization methods could be
ð7:1Þ adopted for high temperature combustion of both TDSS and BDSS
(Tang et al., 2012).
ð7:2Þ
4. Conclusions
This study showed that biodrying of sewage sludge produced
porous BDSS with higher LHV and lower N content than TDSS. In
TG-MS and kinetic analysis, BDSS exhibited higher combustibility
and less production of nitrogenous pollutants compared to TDSS.
In addition, BDSS emitted less CO and NO gases, especially at low
temperatures (800 °C) during isothermal combustion. These
reductions of CO and NO were attributed to the porous structure
of BDSS and N consumption during biodrying. Based on these
results, this study suggested that biodrying could be a beneficial
method providing not only energy saving for water removal which
was essential for sludge derived solid fuel production, but also less
pollutant emissions in subsequent combustion. Moreover, com-
pared to composting and anaerobic digestion, it was expected that
biodrying-combustion might accomplish both energy recovery and
reduction of sludge volume and mass in a shorter time.
10 Z. Hao et al. / Waste Management xxx (2017) xxx–xxx
Acknowledgements
This study was supported by the National Research Foundation
of Korea (NRF) funded by the Ministry of Education, Science and
Technology (2015R1D1A1A01059073). Z. Hao is also grateful for
the support of the China Scholarship Council (No. 201307565002).
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