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• Explore the use of catkins as an additive This work presents studies on the combustion of Composite Biomass Pellets in fluidized bed. The use
to the CBPs fuel and assess its utilization. of catkins as an additive to the CBPs fuel is first time and proved well.
• Combustion of CBPs is a first-order reac-
tion, and it is divided into three stages.
• Combustion of CBPs is mainly focused
on the stage of volatile-release.
a r t i c l e i n f o a b s t r a c t
Article history: This work presents studies on the combustion of Composite Biomass Pellets (CBPS) in fluidized bed using bauxite
Received 19 November 2016 particles as the bed material. Prior to the combustion experiment, cold-flow characterization and thermogravi-
Received in revised form 1 May 2017 metric analysis are performed to investigate the effect of air velocity and combustion mechanism of CBPS. The
Accepted 3 May 2017
cold-state test shows that CBPs and bauxite particles fluidize well in the fluidized bed. However, because of
Available online xxxx
the presence of large CBPs, optimization of the fluidization velocity is rather challenging. CBPs can gather at
Editor: D. Barcelo the bottom of the fluidized bed at lower gas velocities. On the contrary, when the velocity is too high, they accu-
mulate in the upper section of the fluidized bed. The suitable fluidization velocity for the system in this study was
Keywords: found to be between 1.5–2.0 m/s. At the same time, it is found that the critical fluidization velocity and the pres-
Fluidized bed sure fluctuation of the two-component system increase with the increase of CBPs mass concentration. The ther-
Composite biomass pellets mogravimetric experiment verifies that the combustion of CBPs is a first-order reaction, and it is divided into
Characteristics three stages: (i) dehydration, (ii) release and combustion of the volatile and (iii) the coke combustion. The com-
Combustion bustion of CBPs is mainly based on the stage of volatile combustion, and its activation energy is greater than that
of char combustion. During the combustion test, CBPS are burned at a 10 kg/h feed rate, while the excess air is
varied from 25% to 100%. Temperatures of the bed and flue gas concentrations (O2, CO, SO2 and NO) are recorded.
CBPs can be burnt stably, and the temperature of dense phase is maintained at 765–780 °C. With the increase of
the air velocity, the main combustion region has a tendency to move up. While the combustion is stable, O2 and
CO2 concentrations are maintained at about 7%, and 12%, respectively. The concentration of SO2 in the flue gas
after the initial stage of combustion is nearly zero. Furthermore, NO concentration is found to be closely related
⁎ Corresponding authors.
E-mail addresses: kerry151@126.com (F. Guo), zzhong@seu.edu.cn (Z. Zhong).
http://dx.doi.org/10.1016/j.scitotenv.2017.05.026
0048-9697/© 2017 Elsevier B.V. All rights reserved.
F. Guo, Z. Zhong / Science of the Total Environment 599–600 (2017) 926–933 927
to O2: the NO reaches its peak value after initial stage and later decreases with the continued depletion of O2. To-
wards the end of combustion, NO increases with the increase of O2.
© 2017 Elsevier B.V. All rights reserved.
Edited by: D. Barcelo The combustion mechanism of biomass pellets has been studied by
numerous researchers. Li et al. (2012) investigated the reaction mecha-
nism of four typical types of Chinese biomass by TG-DTG and the results
1. Introduction showed the combustion of biomass could be divided into three phases:
(i) water evaporation process, (ii) volatile component combustion pro-
Because of the energy shortage and environmental problems, many cess, and (iii) the fixed carbon combustion process. According to the
researchers are investigating alternative to fossil fuels, where in partic- combustion characteristics of biomass, Demirbas (2004) found that
ular biomass combustion has becomes more attractive (Panoutsou et al., the burning rate of the biomass was much higher than that of coal.
2009; Zeng et al., 2016). Fluidized-bed combustion technology has been Qian et al. (2011) conducted experiments on the NO emission of bio-
proven as one of the most effective technologies for energy conversion mass. It was noted that NO emission decreased with the excess air,
of different kinds of biomass.(Kaynak et al., 2005; Chyang et al., 2008; and increased with the bed temperature. Compared with char-N,
Youssef et al., 2009). Biomass pellets type fuel has high burning efficien- volatile-N is the more dominant reactant source for NO emission.
cy, environmentally friendly, with convenient storage and transporta- Ninduangdee and Kuprianov (2014) determined the best combustion
tion, and can be used in the field of heating, power generation and so and emission performance of the conical fluidized-bed combustor was
on.(Fournel et al., 2015; Nunes et al., 2014; Forbes et al., 2014; Saidur achievable when burning palm kernel shell with a mean particle size
et al., 2011). In this study we focus on China's particle fuel, with a variety of about 5 mm at an excess air of 40–50%. Khan et al. (2009) pointed
of raw materials and relatively wide range of physical and chemical out that the high percentages of alkali (potassium) and chlorine, togeth-
characterizations.(Tian, 2006). The Composite Biomass Pellets (CBPs) er with high ash content, were the major sources of agglomeration
used in this experiment is mainly composed of wood chips, rice straw problems. According the study of Duan et al. (2013) CO emission in-
and Chinese parasol catkins, produced in Nanjing with different supply creased with the in-bed stoichiometric oxygen ratio, but decreased
seasons. There are numerous Chinese parasol trees planted in Nanjing, with excess oxygen ratio.
where every March, under the high temperature and wind condition, Despite numerous research devoted to the biomass study, the mech-
flying catkins seriously affects the lives of the residents (Fig. 1). In this anisms and kinetics of the reactions involved in the combustion of the
study, we are exploring the use of catkins as an additive to the CBPs type of CBPs proposed in this study is not understood as it has not yet
fuel and assess its utilization. been fully investigated.
CBPs are relatively large and can affect the mixing and flow charac-
teristics when blended with the bed materials during fluidization. The
2. PROPERTIES OF CBPs
flow characteristics of biomass particles have been studied by a number
of researchers (Abdullah et al., 2003; Clarke et al., 2005; Cui and Grace,
CBPs are made from wood, rice straw and catkins, with real density
2007; Rao and Reddy, 2010; Si and Guo, 2008; Shao et al., 2013), how-
of about 1100 kg/m3. High density CBPs are easy to store and can be eas-
ever these studies are often based on relatively smaller biomass parti-
ily mixed with the bed materials. As compared with rice husk and straw,
cles with regular shape, such as sawdust, rice husk and straw etc.
the shape of CBPs is cylindrical and the particle size is larger (5–7 mm)
Furthermore, their physical properties and geometric dimensions are
as shown in Fig. 2. Calorific value of CBPs is 17–19 MJ/kg, less than
very different from that of CBPs and the conclusions are not suitable
24.3 MJ/kg of the coal, but more than 13–15 MJ/kg of the straw. Howev-
for the CBPs in this study, hence the fluidization characteristics of CBPs
er, the biomass may contain alkaline that could be a cause of bed
need to be studied.
Fig. 1. Chinese parasol trees in Nanjing. Fig. 2. Photograph of CBPs and three raw materials.
928 F. Guo, Z. Zhong / Science of the Total Environment 599–600 (2017) 926–933
agglomeration (Ma et al., 2016; Gatternig and Karl, 2015; Yu et al., At this velocity, the mass concentration of CBPs at the bottom is greater
2014). For better fluidization, bed materials such as quartz sand or than the upper layers. This is most probably due to the low turbulence
bauxite particles can be mixed with CBPs. In this paper, bauxite particles level at lower speeds, where larger CBPs are less affected by the air
with diameter in the range of 0.5–0.8 mm used as the bed material. The flow and their rise are hindered. With the increase of air velocity, the
actual and bulk density of bauxite is about 2760 kg/m3 and 1180 kg/m3, turbulence intensity increases, and the mass fraction of CBPs becomes
respectively. The proximate and ultimate analyses of CBPs are reported more uniform along the bed height. As can be seen from the chart, as
in Table 1. Generally, CBPs have a high content of carbon and oxygen, the air velocity is increased the mass fraction of CBPs at the bottom of
with a very high level of volatile content. the bed (first floor) is gradually reduced while that of the upper part
(third floor) is gradually increased, leading to an overall distribution
3. Flow characteristics of CBPs balance. At the air velocity of 2.0 m/s, the binary mixture is almost even-
ly distributed in the fluidized bed. Further increase of velocity to 3.0 m/s
3.1. Cold-state experimental apparatus will lead to a decrease of the distribution uniformity of CBPs. This indi-
cates that when the air velocity reaches a certain value, most of the
A cold-state test facility is used to study the mixing properties of CBPs are blown to the upper section of the fluidized bed. However,
CBPs and bauxite particles as sketched in Fig. 3. It mainly consists of a when the flow of air is stopped, the bauxite density is heavy and will
set of air supply devices, a fluidized bed and pressure sensors. The fluid- fall faster than CBPs, thus CBPs tends to be concentrated in the upper
ization reactor is made of Plexiglas and has an overall height of 1.6 m section of the fluidized bed. The similar phenomenon (segregate with
with a cross section of 120 mm ∗ 40 mm. In order to study the flow of smaller denser particles at the bottom, whereas the segregation is in
CBPs in horizontal and vertical direction, first of all, the bed material is the opposite direction at higher superficial velocities) has been well
divided into three layers by two horizontal plates, and then each layer known for liquid-fluidized beds.(Escudié et al., 2006)
is respectively split into three equal parts as depicted in Fig. 3. By this The critical fluidization velocity umf is an important parameter to be
way, the binary mixtures in the whole fluidized bed are divided into measured for the fluidization of different binary mixtures. In this work it
nine grids, and the CBPs content in each section is measured. The air was obtained by recording the corresponding air velocity (u) and pres-
supply system contains roots blower, flow meter and wind chamber. sure drop (△P) while gradually reducing the air velocity until the fluid-
Gas is provided by the air blower and controlled by flow meter. Pressure ized bed slowly restored to a fixed bed. As shown in Fig. 5, at low air flow
signals are monitoring by pressure sensors at the height of 200 mm velocities, the material is in a fixed bed state and the bed pressure drop
above the air distributor. In the experiment, frequency for each mea- is proportional to the air velocity. After further increase of air velocity,
surement is 100 Hz and more than 1024 data are collected every time. the bed begins to expand and produce bubbles, entering into the fluid-
ized phase. After a certain velocity, the pressure drop of the bed layer is
3.2. Experimental method no longer changed. It can be seen from the figure, the critical flow speed
of bauxite alone is 0.6 m/s. The critical fluidization velocity of the mix-
Due to the large size of CBPs, the air mainly flows along the gap be- ture with 10% and 20% of CBPs is 0.65 m/s and 0.71 m/s, respectively.
tween particles, and the CBPs are basically not fluidized. However, the Presence of more CBPs in the mixture will lead to an increase in the crit-
fluidization behavior of CBPs could be improved when they are mixing ical fluidization velocity. At the same time, the total weight of mixtures
with the bed material. Therefore, the mixing characteristics of CBPs in fluidized bed will also increase, leading to a larger corresponding
and bauxite particles are further studied. pressure drop. The pressure fluctuation is also more significant due to
The specific operational procedures are as follows: the binary mix- the existence of higher amount of large CBPs.
tures of CBPs and bauxite particles are added into the fluidized bed
with the initial bed height of 200 mm. The pressure measuring device 4. Thermogravimetric characteristics of CBPs
is opened and the air is injected into the cold-state facility. As the air ve-
locity is increased, the bubbles gradually became larger and led to the 4.1. Experimental method
rise of CBPs and bauxite particles, fluidizing the bed. After 2–3 min,
when the fluidization was stable, the air supply was stopped. The mix- The knowledge of the kinetics of combustion is essential for moni-
tures was divided into nine sections (1–9) by the horizontal plates toring and improving efficiency of commercial combustion. Therefore,
and vertical separators, and, separated by a sieve and weighted. The thermogravimetric (TG) analysis was carried out on the CBP samples
mass fraction of CBPs in nine parts was then obtained to study its mixing in this work. A sample of 18.84 mg CBPs was used for the experiment
behavior. In order to verify the accuracy of experimental data and re- in a SETSYS-1750 CS thermogravimetric apparatus. The air flow was
duce errors, parallel experiments were done for three times and the 20 ml/min, and the heating rate was 20 K/min. The sample was heated
error rate was less than 10%. from 25 °C to 1000 °C, while its weight loss was continuously recorded.
The influence of fluidization velocity on the mixing behavior of CBPs Data from TG and Differential TG (DTG) curves can be used to deter-
has been studied in this work. Fig. 4 shows that when the flow velocity mine the kinetic parameters, which are obtained according to the inte-
is 0.8 m/s, the blending of CBPs and bauxite particles is not satisfactory. gral method of Freeman-Carroll. This method has been successfully
used for studies on the kinetics of decomposition and combustion bio-
mass fuels.
Table 1 The kinetic equation is expressed as:
Properties of CBPs.
Proximate analysis (air dry %) Ultimate analysis (air dry %) da=dt ¼ Ae−E=RT f ðaÞ ð1Þ
Moisture 4.2 Carbon 44.17
Ash 10.1 Hydrogen 5.86
Assuming, f(a) = (1 − a)n and n = 1, is first-order reaction. To bring
Volatile 72.51 Sulfur 0.03
Fixed carbon 13.19 Nitrogen 0.14
it into Formula (1):
Oxygen 40.16
Fig. 3. Schematic diagram of the cold-state fluidized bed. 1-roots blower 2-header 3-rotameter 4-air distribution chamber 5-horizontal plate 6-fluidized bed reactor 7-pressure
measurement points 8-pressure sensor 9-data collector 10-laptop.
Under the condition of linear heating, the heating rate of w = dT/dt is − RE ; x ¼ T1, Formula (4) can be simplified as: y = a + bx. By taking a se-
brought into Formula (2): ries of points on the TG curve, the corresponding y, x value can be calcu-
lated and a straight line can be made by linear regression method, from
A −E=RT
da=dT ¼ e ð1−aÞ ð3Þ which the slope, b, and the intercept, a, can be obtained. At last, the ac-
w
tivation energy E and frequency factor A also can also be calculated.
Eq. (3) can be transformed by the integration as follow:
4.3. Results and discussion
− ln ð1−α Þ AR 2RT E
ln 2
¼ ln 1− − ð4Þ
T wE E RT
In Fig. 6, CBPs combustion is divided into three periods; the first
stage is dehydration from 60 °C to 190 °C; the second stage is
The conversion coefficient a is defined as a = (m0 − m)/(m0 − mF),
190–410 °C for volatile combustion phase in CBPs; the third stage is
where m0 represents the initial mass of the sample; m represents the
410 °C to 590 °C mainly for coke combustion. During the three stages,
sample mass in the experimental process; mF represents the mass of
the TG curve shows three weight loss steps, and the DTG curve repre-
the combustion residue; t represents the reaction time; w represents
sents three peaks of weight loss rate: water loss, volatile release and
the heating rate; A is the pre-exponential factor; E is the apparent acti-
combustion and fixed carbon combustion. The peak of volatile release
vation energy; R is the gas constant (8.314 J/(mol·K); T is the reaction
and combustion is much greater than that of fixed carbon combustion.
temperature.
It is mainly because the mass fraction of volatile is larger than the
For most reactions, 2RT/E is much less than 1, and a ¼ ln ½− ln ð1−αÞ
T2 fixed carbon, so the release and burning rate in second stage is higher.
can be regarded as constant. Then if y ¼ ln ½− ln ð1−αÞ
T2
; a ¼ AR
lnðwE Þ; b ¼ The volatilization of CBPs occurs at about 200 °C, and its combustion
process at the early stages is mainly based on the volatile combustion.
Fig. 4. The effect of air velocity on CBPs mass fraction. Fig. 5. The relationship of pressure drop with air velocity.
930 F. Guo, Z. Zhong / Science of the Total Environment 599–600 (2017) 926–933
Table 3
Combustion kinetic parameters of CBPs.
Fig. 7. Schematic diagram of the combustion experimental set-up. 1-blower 2-header 3-diesel tank 4-diesel combustion chamber 5-screw feeder 6-hooper 7-water cooler 8-fluidized bed
reactor 9-heating jacket 10-heat exchanger 11-fluidized gas inlet12-heating gas inlet 13-primary cyclone separator 14-secondary cyclone separator 15-ash bucket 16-fabric filter 17-
induced draft fan 18-chimney.
2.83 m/s, the temperature in fluidized bed reduced. At this time, some of can easily generate stable inorganic sulfate with alkali metal elements
the bed materials and CBPs are blown out because of high velocity, and at the high temperature as shown below.
the combustion efficiency is reduced.
The analysis of the flue gas is carried out on the gas stream exiting SO2 ðgÞ þ 1=2O2 ðgÞ þ H2 OðgÞ þ 2KClðgÞ→K2 SO4 ðgÞ þ 2HClðgÞ ð5Þ
from fabric filter, where specifically O2, CO, CO2, SO2 and NO concentra-
tions are measured simultaneously with MRU600 gas analyzer for emis- The maximum temperature of biomass combustion is reported to be
sion monitoring and combustion analysis (made in Germany). less than 1300 °C,(Bai et al., 2013; Zhao et al., 2014) hence NO is usually
According to the variations of O2 and CO2 concentrations, as shown in accounted for more than 90% of the total produced NOx.(Wang et al.,
Fig. 9, the combustion process can be divided into: (i) start of combus- 2015) Therefore in this paper we focus on the analysis of NO emission.
tion, (ii) stable combustion and (iii) the end of combustion. Tests with Oxidation of fuel nitrogen, called fuel NO.(Yamamoto et al., 2012) As
continuous feed of biomass are carried out and it is also found that the
discharge of pollutants in steady state is similar to that of in Fig. 9
from 600 s to 800 s. At the beginning of combustion, the O2 concentra-
tion begins to decrease, and the CO2 concentration increases. After
reaching point B, the O2 concentration is maintained at about 7%, and
that of CO2 is 12%, which refers to the stage of stable combustion. At
the start of combustion, the emission concentration of SO2 is
50–60 ppm, caused by incomplete combustion. In the stable phase,
the SO2 of CBPs combustion is very low. The level of pollutant emission
is far lower than that of air pollutant emission standards. It should be
noted that the sulfur content of CBPs is low and in addition, the SO2
Table 4
Operating parameters of CBPs combustion.
1 50 1.25 1.25
2 60 1.50 1.75
3 70 1.75 2.25
4 80 2.0 2.83
Fig. 8. The effect of gas velocities on the bed temperature profiles.
932 F. Guo, Z. Zhong / Science of the Total Environment 599–600 (2017) 926–933
The calculated ratio of B/A for CBPs in this work is 2.12 and higher
than that of coal (B/A = 0.4–0.7) (Yamamoto et al., 2012). Therefore,
the heated surface of CBPs combustion can be easily deposited with
ash, and it is necessary to consider a blowing mechanism on the
heated surface. However, as bauxite is used as the bed material and
its main material is Al2O 3 , the slagging rate can be reduced
significantly.
6. Conclusions
CBPs are composite product of three kinds of biomass, which can po-
tentially solve the problem of raw material supply cycle. Meanwhile, it
will make full use of the Chinese parasol catkins in Nanjing area.
Experimental results suggest the CBPs and bauxite material can mix
and flow together, and the critical fluidization velocity of binary mixture
is about 0.6–0.7 m/s. Optimum fluidization velocity for better mixing of
Fig. 9. The variation of main gas concentrations in the combustion process.
the system was found to be 1.5–2 m/s.
The combustion of CBPs is found to follow a first-order reaction
model, and it can be divided into three stages: (i) dehydration
the fuel type N of CBPs is volatile at high temperature, and the NO is gen- (60–190 °C), (ii) the release and combustion of the volatile (190–410
erated under oxidization conditions. At point A, NO concentration °C) and (iii) the coke combustion (410–590 °C). CBPs can ignite and
reaches the peak of 120 ppm, where the concentrations of O2 and CO2 burnout and the combustion is mainly based on volatile combustion,
are equal. With the continuous depletion of O2, generating more CO where its activation energy is greater than that of char combustion.
and other reducing gases, NO can be reduced to N2 and causes a de- CBPs can burn steadily and in this work the temperature of dense
crease of NO concentration to 40–70 ppm. With the later increase of phase is maintained at 765–780 °C. With the increase of the air velocity,
O2 concentration at the end of combustion NO also increases, shown the temperature in fluidized bed rises, and the temperature difference
in region C in Fig. 9. between dense phase and dilute phase is decreased from 35 °C to 10
The ash fouling rate of CBPs is closely related to its chemical compo- °C, and shows the main combustion region has a tendency to move
sition. The analysis of ash sample from cyclone dust collector and up. O2 concentration is maintained at about 7%, and CO2 is 12%, while
depicted is presented in Fig. 10. The combustion ash is mainly composed the emission concentration of SO2 is nearly zero. NO concentration
of CaO, K2O and SiO2. CaO accounts for 35% of the ash contents. Its higher first rises to the peak value of 120 ppm, but with the consumption of
component content lowers the ash melting temperature. SiO2 and K2O O2, NO decreases to 40–70 ppm, and finally increases again with the in-
account for 16% and 13% of the ash content, respectively and could be crease of O2. The calculated ratio of alkali to acid is 2.12, suggesting the
responsible for agglomeration and heating surface fouling. The reason heated surface of CBPs combustion can be easily deposited, nevertheless
is that alkali metal oxide reacts with SiO2 to produce low temperature bauxite particles which contain most of the bed materials can help with
co-melt, which leads to serious sintering phenomenon in the fluidized the slagging reduction.
bed. In order to characterize the fouling tendency and the fouling rate
of the heated surface during CBPs combustion, the alkali to acid (B/A) Abbreviations
ratio is introduced,(Sun et al., 2010) which is defined as: umf Minimum fluidization velocity
u Superficial air velocity
△P Bed pressure drop
B=A ¼ wðCaOÞ þ wðK2 OÞ þ wðNa2 OÞ þ wðFe2 O3 Þ
þ wðMgOÞ=wðSiO2 Þ þ wðAl2 O3 Þ ð6Þ TG Thermogravimetry
DTG Derivative thermogravimetry
a Conversion coefficient
m0 Initial weight of the sample (mg)
m Actual weight of the sample (mg)
mF Final weight of the sample (mg)
T Absolute temperature (K)
n Reaction order
A Frequency factor (min−1)
E Activation energy (KJ/min)
r Correlation coefficient
XRF X-ray fluorescence
Notes
Acknowledgements
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