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

Analysis of the combustion of sewage sludge-derived fuel by a


thermogravimetric method in China
Jianguo Jiang a,b,*, Xuejuan Du a, Shihui Yang a
a
Department of Environmental Science and Engineering, Tsinghua University, Beijing 100084, China
b
Key Laboratory for Solid Waste Management and Environment Safety, Ministry of Education of China, China

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

Article history: The treatment and disposal of sewage sludge are significant environmental problems in China. The reuse
Received 3 December 2009 of sewage sludge for fuel could be an effective solution. The aim of this study was to characterize the
Accepted 9 March 2010 behavior of sludge-derived fuel during combustion by a thermogravimetric method. The combustion pro-
Available online xxxx
files obtained showed four obvious weight loss regions. The results of dynamics analysis showed that
first-order reactions together with Arrhenius’ law explained reasonably well the different stages of
weight loss in the samples. Three temperature regions (162–327 °C, 367–445 °C, and 559–653 °C for saw-
dust and 162–286 °C, 343–532 °C, and 609–653 °C for coal) in each derivative thermogravimetry (DTG)
curve corresponded well with the Arrhenius equation. The reactivity of sludge was lower than that of
samples containing sawdust, but higher than that of coal-containing samples. These data demonstrate
that sludge-derived fuel has better combustion characteristics than sludge, sawdust, or coal.
Ó 2010 Elsevier Ltd. All rights reserved.

1. Introduction No proper sludge treatments or disposal methods are currently


applied in China. Many wastewater treatment plants accumulate
The treatment and disposal of sewage sludge have become large amounts of sludge which leads to secondary pollution and
environmental problems in China. In 2007, 58 billion tons of sew- environmental and social problems (Wang et al., 2006). As pre-
age drainage were generated in China, representing an increase of scribed by the ‘‘Standard for Pollution Control on the Landfill Site
about 5.9% compared to the sewage drainage in 2006 (Investment of Municipal Solid Waste” (GB16889-2008), only sludge with a
Evaluation Report of the Wastewater Treatment Industry in China water content of less than 60% can enter landfill sites in China. In
2008). The daily sewage processing capacity reached 70 million m3 most of Europe, solid wastes containing biodegradable organic
at the end of 2007, an increase of 10.0% compared to that of 2006; substances are not allowed to enter landfill sites. Denmark and
the treatment rate of city sewage reached 59.0%, an increase of Switzerland implemented this ban on 1 July 1997 and 1 January
3.3% compared to the previous year (Bulletin of National Economy 2000, respectively. In Germany, landfill treatment of sewage sludge
and Society Development of the People’s Republic of China 2007). with an organic substance content above 5% is banned by the
Assuming that 1 ton of sewage sludge with a water content of ‘‘Guide for Treating Technology of Municipal Waste” (Li, 2004;
80% is produced for every 1000 tons of sewage, 26 million tons of Cenni et al., 2001; Zhou, 2003).
sludge were produced in China in 2007, which amounts to an an- Sludge incineration has received worldwide attention as an
nual increase of 10%. effective approach to reduce the quantity and toxicity of sludge
Sewage sludge is a large volume byproduct of city sewage. This and has been applied in Europe, the US, and Japan for many years.
sludge has a high water content, is difficult to dehydrate, and con- However, direct sludge incineration is not cost efficient and creates
tains unstable organic substances that decompose and conse- unstable burning conditions that generate high amounts of gas-
quently create bad odors. Moreover, sewage sludge contains eous pollutants (Liu, 2004; Werther and Ogada, 1999).
toxic pollutants and large amounts of heavy metals. Sewage sludge In order to improve the combustion characteristics of sewage
is also laden with harmful pathogens and parasite ova that threa- sludge, it was mixed with auxiliary fuels, sulfur-fixating agents,
ten the health of human beings (Zhou et al., 2000; Chen and Zhao, and preservatives, and the blends were granulated, generating
2006; Werther and Ogada, 1999). sludge-derived fuel (SDF). Studies by Jiang and Du (2007), Hu
and Hong (1996), Wang et al. (2000), Wang (2002), and Tian
et al. (2000) have made important contributions to understanding
* Corresponding author at: Department of Environmental Science and Engineer- the granulating and combustion characteristics of sewage sludge-
ing, Tsinghua University, Haidian District, Beijing 100084, China. Tel./fax: +86 10 derived fuels. Dospoy et al. (1998) created sewage sludge-derived
62783548.
fuels from paper sludge, coal powder, and plastics and successfully
E-mail address: jianguoj@tsinghua.edu.cn (J. Jiang).

0956-053X/$ - see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.wasman.2010.03.009

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applied them in practical projects. Probst et al. (1995), Folgueras


et al. (2004), and Leckner and Amand (2004) elucidated the emis- 1
sion characteristics of flue gas by incinerating mixtures of sewage
sludge and coal. Furthermore, Otero et al. (2002) and Liu et al.
(2006) analyzed the combustion reaction characteristics of sludge
and sludge-coal mixtures from different sources with the aid of
thermal gravitational analysis (TGA). Wen et al. (2004) studied 2
the combustion weight loss behaviors of sludge from 50 °C to
950 °C at different heating speeds (20 °C/min, 30 °C/min, and 4 3
50 °C/min) by TGA and proposed a combustion dynamics model 5
composed of three independent and continuous parallel reactions.
Most of the former studies used directly the mixture of sludge
and coal. However, in the process of generating SDF, two factors 6
– the additives and the mechanical extrusion – could cause change
in the content and the structure of it, and subsequently cause
change in combustion characteristics. Thus this study, with the
use of thermogravimetric tests and dynamics analysis, investigated
the combustion characteristics of SDF, for the purpose of provide a Fig. 1. The basic structure of the granulator: (1) feeder, (2) roller, (3) flat die, (4)
framework for using sewage sludge-derived fuel in industrial scraping cutter, (5) outlet, and (6) motor.
applications. Besides coal, the influence of another auxiliary fuel
– sawdust – on the combustion characteristics of sludge-derived
fuels was also studied. diameter of the granules can be controlled by exchanging tem-
plates with differently tapped holes.

2. Materials and methods 2.2.2. Analytical methods


The samples were first dried in an oven under 105 °C. The
2.1. Raw materials weight loss divides the mass weight was the water content.
Then the dried samples were sealed in the crucible and heated
The sewage sludge used in these experiments was from the in the muffle under 600 °C for 2 h. The weight loss was the volatile
dehydrating room at the Gaobeidian Wastewater Treatment Plant matter.
in Beijing, China. Sawdust was acquired from a wood processing The samples were put in the muffle under 800 °C in an oxidizing
factory, and the coal was from a coal-fired power plant. The basic atmosphere for 2 h, and the residues were the ashes.
characteristics of the raw materials are shown in Table 1. The The fixed carbon was calculated by 1  the volatiles content and
dry-basis heat value of the sludge was 2591 kcal/kg, which is the ash content.
approximately half of the heat value of coal. The content of fixed Thermogravimetric analysis was done with a METTLER TGA/
carbon in the sludge was as low as 3.48%, while the content of vol- SDTA851e thermogravimetric analyzer. Several granules were ran-
atile matter was as high as 43.67%, which promotes efficient com- domly picked, dried, ground into powder and screened through
bustion of the material. The contents of N, S, and Cl in the sludge 100 mesh screen. Around 10 mg of each sample was then analyzed
were 3.63%, 1.42%, and 0.16%, respectively; these values were high- in the thermogravimetric analyzer with a heating rate of 20 °C/min
er than the corresponding contents in coal and sawdust. from 100 °C to 900 °C under an air flow of 100 mL/min.

2.2. Methods 3. Results and discussion

2.2.1. Briquetting 3.1. Basic characteristic analysis


The sludge was first dehydrated in an oven to a water content of
60% and then mixed with additives according to the proportion- The results of proximate analyses are shown in Fig. 2. Proximate
ing scheme shown in Table 2. The pure sludge and the blends were analysis showed that auxiliary fuels significantly influenced the
then sent into a granulator (Fig. 1), where the derived fuel was pro- sample contents.
duced in bar form, respectively. Subsequently, the granules were As shown in Fig. 2, addition of sawdust reduced the ash content
placed in a well-ventilated area and air-dried for 2 days for later and increased the volatile matter content, but the fixed carbon
analysis. content was not affected significantly. When the proportion of
The granulator applied in this experiment was a flat-die rolling sawdust was increased from 0 to 2, the ash content was reduced
granulator. The operational principle is as follows: the materials from 52.85% to 18.68%, which is 35% of that in sewage sludge.
are added from a feeder, rolled by a high-speed rolling wheel, ex- The volatile matter content increased from 43.67% to 75.72%, the
truded with force from a tapped flat die, and cut off by the scraping fixed carbon content increased slightly from 3.48% to 5.60%, and
cutter under the template, which produces columned granules. The the heating value increased from 2591 kcal/kg to 3433 kcal/kg.

Table 1
Characterization of materials.

Sample Moisture Volatiles Ashes Fixed carbon C (d.b.) H (d.b.) N (d.b.) S (d.b.) Cl (d.b.) HHV (d.b.)
content (%) (d.b.) (%) (d.b.) (%) (d.b) (%) (%) (%) (%) (%) (%) (kcal/kg)
Sewage sludge 73.57 43.67 52.85 3.48 35.08 5.48 3.63 1.42 0.16 2591
Coal 1.75 13.48 26.45 60.07 62.14 – 0.75 – 5212
Sawdust 12.71 82.52 1.38 16.10 50.54 – 0.04 – 4531

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Table 2
Sample composition of sewage sludge-derived fuel in grams. (a) 0.6
Sludge Auxiliary fuels Preservatives Binder agents 0.5

ash content/%
(60% moisture)
Coal Sawdust 0.4
Sludge 400 0 0 8 8
0.3
M2 400 80 0 8 8
coal
M3 400 160 0 8 8 0.2
M4 400 240 0 8 8 sawdust
M5 400 320 0 8 8 0.1
J2 400 0 80 8 8
J3 400 0 160 8 8 0
J4 400 0 240 8 8 0 0.5 1 1.5 2
J5 400 0 320 8 8
ratio of auxiliary fuel to sludge/g·g -1

In contrast, when coal served as the auxiliary fuel, the ash, and (b) 0.9
volatile matter content in the samples decreased slightly, and the 0.8

volatiles content/%
fixed carbon content increased notably. When the proportion of 0.7
coal was increased to 2, the ash content was reduced to 38.84%, 0.6 coal
which is about 70% of that in sewage sludge. Using this proportion 0.5 sawdust
of coal decreased the volatile matter content to 35.49%; the fixed 0.4
carbon content increased to 25.67%, and the heating value in-
0.3
creased to 4029 kcal/kg.
0.2
0.1
3.2. Combustion performance analysis 0 0.5 1 1.5 2
ratio of auxiliary fuel to sludge/g·g -1
Fig. 3 shows the combustion curves – weight loss curves (TG)
and weight loss rate curves (DTG) – of sewage sludge and other (c) 0.3
samples. As shown in Fig. 3b and d, each of the DTG curves from coal
(b)
all samples had four peaks, representing the water content sepa- fixed carbon content/% 0.25 sawdust
rating phase, the emanation of volatile matter, the combustion of 0.2
volatile matter, and the combustion of fixed carbon. The burning
profiles for the samples using the two different auxiliary fuels 0.15
are shown. 0.1
In Fig. 3b, sawdust dose-dependently increased the weight loss
speed of the second phase compared to the third phase; increased 0.05
quantities of sawdust increased the difference between the weight 0
loss speed phases. The onset temperature for volatile release and 0 0.5 1 1.5 2
weight loss of all samples were close. However, as the proportion ratio of auxiliary fuel to sludge/g·g-1
of sawdust increased, the maximum weight loss rate in volatile re-
lease phase increased notably, and the combustion of volatiles
started earlier. In the forth phase, the combustion of fixed carbon
(d) 5000
started at lower temperature when sawdust added.
heating value/kcal·kg-1

4000
In contrast, when coal was used, the weight loss speed of the
second phase was notably lower than that of the third phase, and 3000
increased quantities of coal decreased the weight loss speed in
2000 coal
the second phase and increased the weight loss speed in the third
phase. As the increase of coal proportion, the maximum weight sawdust
loss rate of volatiles decreased gradually and the combustion 1000
started later.
0
0 0.5 1 1.5 2
3.3. Dynamics analysis
ratio of auxiliary fuel to sludge/g·g -1
The kinetic equation of the combustion process of each sample Fig. 2. The results of proximate analyses for the samples: (a) ash content; (b)
can be expressed as follows (Qin et al., 2004): volatiles content; (c) fixed carbon content; and (d) heating value.

da
¼ kf ðaÞ;  
dt da E
¼ kf ðaÞ ¼ A exp  ð1  aÞn ;
where a is the conversion rate of combustion products or the weigh dt RT
loss rate of the samples in this experiment, t is the time, and k is the
reaction rate constant. and calculation of the natural logarithm of both sides yields
Assuming that the combustion reaction is an nth-order simple
reaction, then  
da E
n ln ð1  aÞn ¼ þ ln A:
f ðaÞ ¼ ð1  aÞ : dt RT
 
Application of the Arrhenius equation over the above formulas Let Y ¼ ln ð1  aÞn ddta , and X ¼ T1, and the above equation can
gives be expressed as a linear equation as follows:

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Fig. 3. TG and DTG curves for the samples: (a) weight loss curves for samples added coal; (b) weight loss rate curves for samples added coal; (c) weight loss curves for
samples added sawdust; and (d) weight loss rate curves for samples added sawdust.

E well with the Arrhenius equation. The durations were 5.61 min,
Y ¼  X þ ln A:
R 3.49 min, and 2.17 min, respectively, and the weight loss rates
The combustion of the samples can be recognized as a series of were 10.1%, 9.2%, and 2.1%, respectively. The correlation coeffi-
first-order reactions. From the TG and DTG profiles, the tempera- cients of the linear fitting equations of the three phases were all
ture, sample weight, and weight loss rate at any time can be ob- above 0.97. The data obtained show that each of the Y–X curves
tained, and the corresponding Y and X can be calculated. Take of all samples has three lines with negative slope during the heat-
sludge as an example, using the data obtained from the TG and ing process, fitting well with the Arrhenius equation in three
DTG profiles, Y and X can be calculated. In the Y–X curve, there phases (Fig. 4). The activation energy, E, and the frequency gene,
are three lines with negative slope. These three phases of sludge A, can be calculated by linear fitting. Table 3 shows the kinetic
are 162–274 °C, 367–437 °C, and 609–653 °C, which fit relatively parameters of all samples.

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(a) 4.0
sludge
3.5 J5
J4
3.0
J3
J2
2.5

2.0
ln (k)

1.5

1.0

0.5

0.0
0.0010 0.0012 0.0014 0.0016 0.0018 0.0020 0.0022 0.0024
-0.5
1/T

(b) 3.0 sludge


M5
2.5 M4
M3
2.0 M2

1.5
ln (k)

1.0

0.5

0.0
0.0010 0.0012 0.0014 0.0016 0.0018 0.0020 0.0022 0.0024

-0.5

-1.0
1/T

Fig. 4. Arrhenius plots for the combustion of different samples: (a) samples added coal and (b) samples added sawdust.

When sawdust served as the auxiliary fuel, the starting temper- When coal was adopted as the auxiliary fuel, the first phase
ature of the first phase was 162–171 °C, and the end-point temper- starting-point and end-point temperatures were 162–194 °C and
ature was 274–327 °C. As the proportion of sawdust increased, the 274–286 °C, respectively. With increased proportions of coal dust,
duration rose from 5.61 min to 8.22 min, and the weight loss rate the weight loss rate fell from 10.l% to 3.8%. In the second phase, the
increased from 10.1% to 37.8%. For the second phase, the start- starting-point and end-point temperatures were 343–400 °C and
ing-point and end-point temperatures were 367–375 °C and 407– 437–532 °C, respectively. As the proportion of coal dust increased,
445 °C, respectively. The duration increased from 1.68 min to the duration rose from 3.49 min to 9.35 min, and the weight loss
3.51 min, and the weight loss rate also increased from 5.8% to rate increased from 9.2% to 37.5%. In the third phase, the start-
9.2%. The beginning and end temperatures for the third phase were ing-point and end-point temperatures were 609–621 °C and 640–
559–609 °C and 627–653 °C, respectively; the duration increased 653 °C. As the proportion of coal dust increased, the duration rose
from 2.15 min to 3.36 min, and the weight loss rate rose from from 1.04 min to 2.17 min, and the weight loss rate increased from
1.3% to 2.1%. 0.8% to 2.1%.

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Table 3
Kinetic parameters of the samples.

Samples Stage Ei (J/mol) Ai (min1) R2 Starting-point End-point


Time (min) Temperature (°C) Weight (%) Time (min) Temperature (°C) Weight (%)
Sludge 1 39,471 5.2E+04 0.9925 7.67 162 98.9 13.28 274 88.8
2 28,712 8.0E+02 0.9584 17.94 367 75.5 21.43 437 66.3
3 165,881 1.5E+10 0.9532 30.05 609 57.9 32.21 653 55.8
J2 1 48,009 4.2E+05 0.9906 7.29 169 98.4 14.70 317 72.8
2 27,744 1.2E+03 0.9652 17.56 374 58.1 19.24 407 52.3
3 212,938 1.7E+13 0.9632 28.65 596 38.5 30.80 639 36.9
J3 1 54,957 2.5E+06 0.9929 7.22 167 98.8 14.95 321 67.3
2 26,514 1.4E+03 0.9778 17.45 371 50.7 19.44 411 42.4
3 199,395 3.1E+12 0.9621 28.65 595 27.1 30.87 640 25.8
J4 1 56,001 2.9E+06 0.9942 8.10 171 98.7 15.70 323 66.5
2 26,616 1.3E+03 0.9290 18.47 378 48.2 20.53 419 39.1
3 188,902 8.5E+11 0.9645 28.69 583 26.0 31.15 632 24.6
J5 1 54,454 2.3E+06 0.9922 7.55 162 99.1 15.76 327 61.3
2 30,689 4.1E+03 0.9874 18.19 375 43.0 21.70 445 25.3
3 131,037 3.5E+08 0.8988 27.40 559 19.1 30.75 627 17.6
M2 1 46,124 1.9E+05 0.9886 9.00 194 98.1 13.37 281 90.4
2 41,944 5.6E+03 0.9808 19.35 400 77.1 25.62 526 58.0
3 190,191 4.5E+11 0.9742 29.95 613 49.4 31.80 650 47.8
M3 1 41,798 4.6E+04 0.9820 7.21 166 99.0 13.10 284 92.5
2 39,835 5.3E+03 0.9358 16.18 345 85.8 25.23 527 54.7
3 230,082 1.4E+14 0.9332 29.52 613 44.1 30.99 642 42.9
M4 1 42,243 3.8E+04 0.9793 8.35 192 99.0 12.92 284 94.6
2 46,711 1.9E+04 0.9577 15.96 345 89.5 25.31 532 53.1
3 219,598 3.2E+13 0.9128 29.66 619 41.9 30.70 640 41.1
M5 1 46,982 9.6E+04 0.9766 9.16 193 99.2 13.81 286 95.4
2 49,272 3.1E+04 0.9615 16.69 343 91.0 25.94 528 53.4
3 199,752 1.6E+12 0.9553 30.55 621 40.4 31.72 644 39.6

As sawdust added, the starting temperature increased slightly in respectively, and the activation energy and the frequency gene of
the second stage, but decreased notably in the third stage, from the first and second stages were 62.3 kJ/mol, 2.3E+5 min1, and
609 °C to 559 °C. The ending temperature in the third stage de- 56.5 k J/mol, 1.2E+3 min1. As the increase of coal, E and A were
creased from 653 °C to 627 °C, indicating that the samples can be not accordingly affected. Comparing to the results in this paper,
incinerated under lower temperature. As coal added, the starting the kinetic parameters of combustion process of different sludge
temperature of the first stage increased significantly from 162 °C varies significantly. The combustion characteristics are relevant
to 193 °C. The ending temperature in the third stage decreased from to the content and also to the structure of the samples. The com-
653 °C to 644 °C. These data showed that the combustion character- bustion characteristics of coal and sludge blends (Folgueras et al.,
istics of the samples were significantly influenced by the addition of 2004; Liu et al., 2006) are quite different from the SDF made by
auxiliary fuel. The sawdust includes more volatiles, while the coal in- coal and sludge.
cludes more fixed carbon. The more the volatile matter is, the easier
the samples can be ignited. The more the fixed carbon is, the more 3.4. Reactivity assessment by weighted mean activation energy
furious the combustion can be and also the more energy can be ob-
tained (Guan, 2008). The decrease of the ending temperature in Cumming (1984) put forward the concept of the weighted mean
the third stage suggests that SDF can be burnt under lower activation energy, namely,
temperature.
As shown in Table 3, the reactivity of the sample increased with Em ¼ F 1 E1 þ F 2 E2 þ    þ F i Ei þ    ;
increased quantities of sawdust added to the fuel; J5 was the most
where Em is the weighted mean activation energy, F i is the matter
reactive sample at all three stages. In contrast, addition of coal de-
quality percentage of the action in some phase, and Ei is the activa-
creased the reactivity of the samples, and in this group the sludge
tion energy for the phase. F i is calculated from Table 3, and Ei is
itself was most reactive. By Folgueras et al. (2004), sludge, coal, and
shown in Table 3. The weighted mean activation energy of the sam-
their blends were tested. In the Arrhenius plot for each type of
ples can be then calculated accordingly (Fig. 5). When the propor-
sludge and its blends with coal, there are two wide regions of lin-
tion of sawdust increased from 0 to 2, the weighted mean
earity in which sludge is the most reactive material. These results
activation energy increased 2.75-fold from 10,153 J/mol to
are consistent with the findings in this paper.
27,960 J/mol. When the proportion of coal added to the sludge in-
By Liu et al. (2006), the ash, volatile matter, and fixed carbon
creased from 0 to 2, the weighted mean activation energy increased
content of sludge used were 54.09%, 38.23%, and 2.88%, respec-
2.16-fold from 10,153 J/mol to 21,907 J/mol. Therefore, the
tively, which were close to the content of sludge in this paper.
weighted mean activation energy of the sludge fuel with sawdust
The starting temperature of the three stages were 215 °C, 430 °C,
was higher than that of the sludge fuel with coal.
and 712 °C, and the activation energy and the frequency gene of
the first and second stages were 41.783 kJ/mol, 7E+3 min1, and
46.377 kJ/mol, 2E+3 min1, respectively. As the increase of coal, E 4. Conclusions
and A of the first stage decreased, while E and A of the second stage
increased. By Folgueras et al. (2004), the ash, volatile matter and A series of thermogravimetric tests on sludge-derived fuel were
fixed carbon content of F sludge were 49.6%, 44.0%, and 6.4%, performed with different ratios of sludge to coal/sawdust. Combus-

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Acknowledgement Beijing.

The authors gratefully acknowledge the ‘‘National Water Body


Pollution Control and Remediation” (No. 2008ZX07313) program
that financially supported this study.

Please cite this article in press as: Jiang, J., et al. Analysis of the combustion of sewage sludge-derived fuel by a thermogravimetric method in China. Waste
Management (2010), doi:10.1016/j.wasman.2010.03.009

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