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The effects of coal blending on the formation and properties of particulate


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Article  in  Chinese Science Bulletin · October 2010


DOI: 10.1007/s11434-010-3250-z

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Article
SPECIAL TOPIC: Huazhong University of Science and Technology October 2010 Vol.55 No.30: 3448−3455
Engineering Thermophysics doi: 10.1007/s11434-010-3250-z

The effects of coal blending on the formation and properties of


particulate matter during combustion
ZHOU Ke, XU MingHou*, YU DunXi, WEN Chang, ZHAN ZhongHua & YAO Hong
State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

Received October 10, 2009; accepted February 9, 2010

The control of particulate matter (PM) emissions from coal combustion becomes an urgent work due to their adverse effects on
human health. Coal blending is a promising option for submicron particulate (PM1) reduction. This study addressed the effects of
coal blending on the formation and properties of particulate matter in combustion process. Coal blends from lignite and bitumi-
nous coal, with different blend ratios (9:1, 7:3, 5:5, 3:7 and 1:9), were combusted in a drop tube furnace. The mass size distri-
bution, concentration, elemental composition and morphology of the particulate matter generated under O2/N2 and O2/CO2 condi-
tions were characterized. Particulate matter was collected by a low pressure impactor (LPI), which aerodynamically segregated
particulates into thirteen fractions with sizes ranging from 0.03 to 9.8 μm. The results showed that coal blending reduced PM1
generation, compared with the calculated average values from the combustion of constituent coals. This indicated that the mineral
interactions had a great effect on PM1 reduction. The blend ratio also played an important role in the suppression of PM1 genera-
tion. In this experimental study, PM1 generation suffered a maximum suppression at the blend ratio of 7:3. The O2/CO2 atmos-
phere affected the formation and properties of the PM1 during coal blends combustion. Compared with the O2/N2 combustion, the
interaction of minerals was weakened under O2/CO2 combustion, thus the suppression of PM1 generation decreased after coal
blending. Compared with the calculated values, the concentrations and percentages of Ca, Fe in PM1 decreased, but the concentra-
tions of Ca, Fe, Si and Al in coarse particulates (PM10+) increased after coal blends combustion. The interactions between the
aluminosilicates in the bituminous coal and volatile elements Ca, Fe in the lignite were thought to contribute to the suppression of
PM1 generation during the combustion of coal blends.

coal combustion, coal blending, particulate matter, O2/CO2 combustion, mineral interaction

Citation: Zhou K, Xu M H, Yu D X, et al. The effects of coal blending on the formation and properties of particulate matter during combustion. Chinese Sci Bull,
2010, 55: 3448−3455, doi: 10.1007/s11434-010-3250-z

The emissions of the inhalable particulate matter (PM10) nisms include: (1) vaporization and subsequent condensation
from coal-fired power plants, especially the submicron of volatile elements [3,4]; (2) the fragmentation of excluded
particulates (PM1) rich in toxic heavy metals, would not minerals [5]; (3) the coalescence of included miner- als [6−8];
only cause the fouling and corrosion of the boiler, conse- (4) char fragmentation [9,10]. The vaporization-condensation
quently affecting the safe operation of boiler and the effi- mechanism is the most important way to form the PM1. Pre-
ciency of heat exchanger, but also harmful to human vious studies [11,12] showed the genera- tion of PM1 was
health and environment [1,2], so more attention has been significantly affected by the coal type, com- bustion tem-
paid to the formation and control technology of coal-de- perature, atmosphere, etc. Buhre et al. [11] showed that the
rived particulate matter. In recently years, the PM forma- lower rank coals had higher submicron ash yields than the
tion mechanisms during individual coal combustion have higher rank coals. Quann and Sarofim [12] found that both
been studied extensively. The major PM formation mecha- high combustion temperature and strong re- ducing atmos-
phere promoted the generation of PM1.
*Corresponding author (email: mhxu@mail.hust.edu.cn) Major control methods of fine particulates from coal-

© Science China Press and Springer-Verlag Berlin Heidelberg 2010 csb.scichina.com www.springerlink.com
ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30 3449

fired plants could be divided into pre-combustion control, proximate and ultimate analysis, as well as the low tempera-
control in the furnace and post combustion control. The ture ash composition of XLT and DT are given in Table 1.
pre-combustion control always refers to the optimization of The ash composition of these two coals varies significantly.
coal characteristics before the pulverized coal enters the Coal XLT mainly contains elements S, Ca, Fe and Coal DT
furnace, such as physical coal washing to remove minerals mainly contains elements Si, Al and S. The blend ratios of the
in coal [13], mixing additives [14], etc. The control in fur- coal XLT/DT are 9:1, 7:3, 1:1, 3:7 and 1:9 by weight re-
nace refers to the optimization of coal combustion condi- spectively. In order to make sure the coals were blended uni-
tions, such as changes in the combustion atmosphere or formly, the ash composition of the coal blends was also ana-
temperature [15,16]. The post combustion control usually lyzed. The results showed that the ash composition of the
refers to adopting the agglomeration or adsorption method coal blends matched their corresponding calculated values,
[17−19] to convert the small particles generated into larger which indicated that the coals were blended uniformly.
ones, which would improve the collection efficiency of
electrostatic precipitators, reducing its emissions to the at- 1.2 Experiment equipment and condition
mosphere. Because of the poor feasibility or high cost, few
PM control methods were used in industrial application, Coal combustion experiments were conducted in an electri-
most of which were still studied in the laboratory. As the cally heated drop tube furnace (DTF). The details of this
coal shortage always puzzled the coal-fired plants, various experimental system can be seen in the literature [25]. A
coals different from the design coal were combusted. In Model MFEV-10 Micro Feeder (Sankyo Piotech Co., Ltd.)
order to stabilize the operation of boilers, coal blending is was used for feeding coal samples with primary gas into the
widely used. Previous researches had shown that [20−22], furnace continuously and constantly. The secondary gas was
blending coal appropriately can reduce the generation of used for complete combustion of coal samples. The particle
fine particulate matter effectively during coal combustion. residence time in the furnace is about 2 s. The particulate
As for different methods of blending coal, the PM reduction matter generated during combustion was collected by a wa-
mechanism is different, so more work should be done to ter-cooled sampling probe with dilution by N2 gas at the
study it in-depth. probe tip, and then introduced into a cyclone which re-
O2/CO2 combustion is an advanced combustion technol- moved the particulate matter with an aerodynamic diameter
ogy used to reduce CO2 emissions from power plants. Re- larger than 10 μm, and finally entered the LPI. The LPI can
cently, the studies by Suriyawong et al. [23] and Sheng et al. separate the particles into 13 fractions with aerodynamic
[24] have found that, compared with the air combustion, diameters ranging from 0.03 to 9.8 μm. In order to ensure
O2/CO2 combustion can also reduce the formation of par- the accuracy of the experiment, the particulate matter sam-
ticulate matter effectively. This is another new approach to
control the emission of submicron particulate matter during Table 1 Properties of raw coal samples
the coal combustion. Nevertheless, there is still a lack of
studies on the control mechanism of the fine particles dur- Properties XLT DT
Proximate analysis (wt%, ad)
ing coal combustion. Particularly, the combined effects of
Moisture 15.5 1.8
blending coal combustion and O2/CO2 combustion on the Volatile matter 45.8 27.8
fine particulates generation is not known. More experiments Ash 15.6 26.6
and further research should be done. Fixed carbon 23.1 43.8
In this paper, lignite and bituminous coal, with different Ultimate analysis (wt%, ad)
mineral compositions, were blended with different ratios C 44.2 55.0
and combusted under different combustion atmospheres. In H 5.7 3.3
order to study the effects of blending coal combustion under S 1.2 0.9
the O2/N2 and O2/CO2 atmospheres on the formation and N 3.2 1.6
characteristics of particulates generated, the size distribution, O (calculated) 14.6 10.8
Composition of low temperature ash (wt%)
concentration, elemental composition and morphology of
Na2 O 2.0 0.1
the particulate were characterized.
MgO 2.8 0.3
Al2 O3 10.0 33.7
SiO2 14.2 42.8
1 The experiment
P2O5 0.8 0.3
SO3 43.1 18.0
1.1 Coal sample
K2O 0.4 0.1
Coal samples, including lignite XLT, bituminous coal DT, CaO 20.5 0.9
and their blends with various blend ratios, with a size of MnO 0.0 0.1
Fe2 O3 6.2 3.7
smaller than 200 μm, were used for the experiment. The
3450 ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30

ples generated under the same condition were sampled at volatile elements.
least three times. It can be seen from Figure 1(b), the coal type affected the
To study the effects of O2/N2 and O2/CO2 combustion on concentration of particulate matter significantly. Under the
the formation of particulate matter from the coal blends same combustion condition, lignite XLT generated more
combustion, a 20% O2 concentration in each combustion PM1 and PM1-10 than coal DT. This is because a consider-
atmosphere was adopted. The furnace temperature is kept at able portion of mineral elements is supposed to exist as or-
1300°C and the feeding rate of the coal powder is about 0.3 ganically bound materials in the lignite XLT, which is easy
g/min. to vaporize. In contrast, coal DT is a bituminous coal, the
main elements exist as inorganics, such as aluminosilicate,
1.3 Sample analysis which is relatively more difficult to vaporize and fragmen-
tize. Therefore, more PM1 and PM1-10 were generated from
The mass size distribution and concentration of the particu- coal XLT combustion than those from coal DT combustion.
late matter is obtained by gravimetric analysis using a Sar- Further discussion will be given combined with the ele-
torius M2P Microbalance (0.001 mg). The particulates col- mental analysis of the particulates. Figure 1(b) also shows
lected by the LPI and cyclone were subject to X-ray fluo- that, compared with O2/N2 combustion, the generation of
rescence spectrometry (XRF) analysis. The particulate PM1 and PM1-10 reduced under the O2/CO2 combustion. As
composition of major elements Si, Al, Mg, Ca, Fe, Na, K, S, these experiments were conducted in the electrically heated
Mn and P were measured. For morphological characteriza- furnace, the gas temperature of the O2/CO2 and O2/N2 at-
tion, particulates collected by the LPI were analyzed under a mospheres were almost the same, no significant effect of the
Fei Sirion 200 field emission scanning electron microscope differences between the CO2 and N2 in specific heat capac-
(FESEM) equipped with energy dispersive spectroscopy ity on the surface temperature of the burning mineral parti-
(EDS). cles. Since the mass and thermal diffusivity of O2 to particle
surface is an important factor affecting the surface tem-
2 Results and discussion perature of the burning coal particles, the mass and thermal
diffusivity of O2 in CO2 smaller than that of O2 in N2 would
2.1 Characteristics of particulate matter generated lead to lower temperature of the burning coal particles un-
from individual coal combustion der O2/CO2 combustion atmosphere [23]. The drop tube
furnace experiment results from Bejarano and Levendis
The PM mass size distributions (a), PM concentrations (b), showed that the particle burning temperature in O2/CO2
and the elemental composition of PM1 (c) and PM1-10 (d) from atmosphere was about 200 K, lower than that in O2/N2 at-
the combustion of coal XLT and coal DT under O2/N2 and mosphere [27]. So when coal combusted under the O2/CO2
O2/CO2 atmospheres are displayed in Figure 1(a)−(d). It is combustion, the vaporization and fragmentation of the min-
showed from Figure 1(a) that, the particulates from coal erals would be suppressed, then the generation of PM1 and
combustion were tri-modally distributed, no matter what kind
PM1-10 was reduced.
of coal it is or what kind of combustion atmosphere it is in.
Figure 1(c)−(d) displays the elemental compositions of
Fine mode particulates centered at the size of 0.1−0.3 μm, is
PM1 and PM1-10 generated from different coals and combus-
mainly formed by vaporization, nucleation and condensation;
tion atmospheres. Under the O2/N2 condition, the PM1 of
while the coarse mode, located in the range of larger than 10
coal XLT mainly contains the elements of Fe, Ca and S.
µm, is usually formed by the excluded mineral fragmentation
and the included mineral coalescence. The central mode cen- This is not only related to the high content of the element Fe,
Ca and S in coal XLT, but also possibly because a consid-
tered at 2.0 μm does not have an agreed formation mecha-
nism yet. Heterogeneous condensation of vaporized species erable portion of Fe, Ca exists as organic forms or carbonate,
on the existing ash particles, as well as char fragmentation, is which is easy to vaporize. Although high Fe content in PM1
suspected to be the main formation mechanisms of the central was unusual, depending on the coal type, similar results
mode particulates [3,10]. It also can be seen from Figure 1(a) were found by Linak and Miller from the combustion of
that, the peak size of the fine mode under the O2/CO2 com- lignite [28]. PM1 from coal DT mainly contains the ele-
bustion is smaller than that under O2/N2 combustion. This is ments of Na, Si and S. Compared with the O2/N2 combus-
consistent with the results of Suriyawong et al. [23] and Sheng tion, the percentage of element Fe in PM1 shows a rapid
et al. [24]. The less growth time for the fine particulates during decrease under the O2/CO2 combustion, indicating that the
the formation processes under the O2/CO2 combustion was decrease in particle combustion temperature has greater
used to explain this phenomenon by Suriyawong et al. [23]. impact on the vaporization of Fe. It also can be seen from
But from the results of other coal combustion experiments Figure 1(d) that the PM1-10 from coal XLT mainly contains
under O2/CO2 atmosphere [26], no similar phenomenon was the elements of Fe, Ca, Si, Al, and PM1-10 of coal DT
found. This result is supposed to relate to the composition of mainly contains the elements of Si and Al. O2/CO2 combus-
minerals in coal, especially the types and existence of the tion has little effect on the composition of PM1-10.
ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30 3451

Figure 1 Characteristics of particulate matter generated from individual coal combustion. (a) PM mass size distributions; (b) PM concentrations; (c) ele-
mental compositions of PM1; (d) elemental compositions of PM1-10.

2.2 Characteristics of particulate matter generated of PM1 was suppressed after the coal blending and the in-
from coal blends combustion teractions between the minerals of these two coal reduced
the generation of PM1. It also can be seen from Figure 2 that
From the results obtained above, it can be seen that different the particulates from the coal blends were still tri-modally
mineral compositions of the coals would result in different distributed, and the peak size of fine mode under the
characteristics of particulate matter generated. To study the O2/CO2 combustion is smaller than that under O2/N2 com-
effects of coal blending on the characteristics of the par- bustion. That is to say, coal blending combustion does not
ticulate matter generated, the comparison between the cal- change the PM formation mechanisms. By comparing the
culated value (Cal.) and experimental data (Exp.) of the differences between the calculated curves and the experi-
mass size distribution, concentration and elemental compo- mental curves with different blend ratios, the experiment
sition of the particulate generated will be studied in detail. results of the different blend ratios leading to different sup-
The calculated values were obtained by eq. (1): pression degrees of the PM1 generation were investigated,
Calculated value=Experimental data (XLT)×Percentage which will be discussed below.
(XLT) + Experimental data (DT)×Percentage (DT). (1) (2) PM concentration. Figure 3 shows the concentration
of PM generated from coal blends combustion with differ-
(1) The mass size distribution. The mass size distribu- ent blend ratios. Figure 3(a) represents the PM concentra-
tions of the PM generated from the combustion of coal tion under O2/CO2 atmosphere, and Figure 3(b) shows the
blends with different blend ratios are shown in Figure 2. PM concentration under O2/N2 atmosphere. Compared with
The comparisons between the calculated particle size dis- the calculated values, the experimental values of PM1 and
tribution curves and the experimental particle size distribu- PM1-10 concentrations reduced after coal blends combustion.
tion curves have been conducted here. It can be seen from Here, the reduction mechanism of PM1 was analyzed. Since
Figure 2, the experimental particle size distribution curves the vaporization-condensation is the major formation
are almost lower than the calculated particle size distribu- mechanism of PM1, the above result indicates that less ele-
tion curves, particularly in the size range of 0−1 μm. It indi- ment vaporized or condensed to form PM1 after the coal
cates that, compared with the calculated value, the generation blends combustion. From the experimental results of the
3452 ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30

Figure 2 The mass size distributions of PM from coal blends with different blend ratios. (a) Blend ratio=9:1; (b) blend ratio=7:3; (c) blend ratio=1:1; (d)
blend ratio=3:7; (e) blend ratio=1:9.

individual coal combustion, it is found that coal XLT pro- suppressed the generation of the PM1. In order to study the
duced more PM1 and PM1-10 than coal DT. The elements Fe, effects of the blend ratio on the suppression degree of PM1,
Ca and S are the main components of PM1 from coal XLT, Figure 4 gives the suppression degrees of PM1 with different
and the elements Si and Al are the main components of blend ratios under O2/N2 and O2/CO2 atmosphere. The sup-
PM1-10 from coal DT. It is expected that the elements Fe, Ca pression degrees of the PM1 were obtained by the eq. (2):
and S from XLT reacted with the aluminosilicates in coal DT Suppression degree=100%−100%× PM1 concentration from
during the coal blends combustion, which leads to the de- coal blends combustion/ PM1 calculated value. (2)
crease of the vaporization of the elements Fe, Ca and S, thus It can be seen from Figure 4 that, the suppression degrees
ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30 3453

of PM1 show a trend of first increase and then decrease with


the increase of the weight percentage of coal DT in the coal
blends. During these experiments, when the blend ratio is 7:3,
the PM1 generation achieved the maximum suppression de-
gree. Compared with the calculated values, the concentrations
of PM1 generated under O2/N2 and O2/CO2 atmospheres were
reduced by 37.8% and 23.3%, respectively. With the weight
percentage of coal DT in coal blends increased, the elements
Fe, Ca and S in coal blends decreased and the elements Si, Al
increased, thus the generation of PM1 would achieve the
maximum suppression when the mole ratio of the volatile
elements Fe, Ca and S to aluminosilicates in coal blends
equaled to the chemical equivalent ratio between them. In the
present study, the blend ratio 7:3 is probably the closest point
equaled to the chemical equivalent ratio.
It also can be seen from Figure 4 that, with the same Figure 4 Suppression degrees of the PM1 with different blend ratios.
blend ratio, the suppression degrees of the PM1 generated
from coal blends under O2/CO2 atmosphere were smaller than
that under O2/N2 atmosphere, mainly due to the lower particle of temperature would weaken the chemical reaction between
surface temperature under O2/CO2 combustion atmosphere. the volatile elements and aluminosilicates. So compared with
On the one hand, the decrease of temperature would lead to O2/N2 combustion, the PM1 from coal blends achieved a
the decrease of elements vaporization, thus reduce their reac- lower reduction under O2/CO2 combustion.
tions with aluminosilicates. On the other hand, the decrease (3) Elemental composition. The interactions between
the volatile elements from coal XLT and the aluminosili-
cates from coal DT were thought to be the main reason for
PM1 reduction during coal blend combustion. In order to
demonstrate it clearly, Figure 5 and Figure 6 show the cal-
culated values and experimental data of the elemental com-
positions and typical elements (Al, Si, Ca and Fe) concen-
trations of the PM generated under O2/N2 atmosphere when
the blend ratios are 7:3 and 3:7, respectively. As Figure 5
shows, compared with the calculated values, the percent-
ages of Ca and Fe in PM1 were reduced and the percentages
of Si, Al and other elements increased in varying degrees,
the percentages of Al, Ca and Fe in PM1-10 increased
slightly after coal blends combustion. It can be seen from
Figure 6 that, compared with the calculated values, the
concentrations of elements Ca and Fe in PM1 were reduced
significantly and no clear changes in the concentrations of
Si and Al after coal blends combustion. The concentration
changes of the elements in PM1-10 based on the calculated
values had a certain relationship between the blend ratios,
when the blend ratio is 7:3, the concentrations of the ele-
ments Al, Si, Ca and Fe were decreased significantly, but
when the blend ratio is 3:7, these changes are not obvious.
The concentration reduction degree of the elements in PM
was affected by the blend ratio. By comparing Figure 5(a)
and Figure 5(b), or Figure 6(a) and Figure 6(b), it can be
found that, when the blend ratio is 7:3, the reduction degrees
of the elements Ca and Fe in PM1 and PM1-10 were always
larger than those under the blend ratio of 3:7. It can be seen
from Figure 5(a) and Figure 6(a), compared with the calcu-
lated value, both the concentration and percentage of Ca and
Figure 3 PM concentrations with different blend ratios. (a) O2/CO2 at- Fe in PM1 decreased, the concentration of Ca and Fe in
mosphere; (b) O2/N2 atmosphere. PM1-10 decreased, and the total concentration of the elements
3454 ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30

Figure 5 Elemental compositions of the PM1 and PM1-10. (a) Blend ratio=7:3; (b) blend ratio=3:7.

Figure 6 Typical elements (Al, Si, Ca, Fe) concentrations in PM1 and PM1-10. (a) Blend ratio=7:3; (b) blend ratio=3:7.

Al and Si in the PM10 decreased after the coal blends com- Fe reacted with aluminosilicates to form more coarse par-
bustion. So the concentration of the elements Al, Si, Ca and ticulates during the coal blends combustion, thereby reduc-
Fe in PM10+ increased. It indicates that some of the elements ing the generation of fine particulate matter.
Al, Si, Ca and Fe were transformed into coarse particles
(PM10+) after the coal blends combustion, which also vali-
dated the interactions between the volatile elements Ca, Fe 3 Conclusions
and aluminosilicates, thereby reducing the generation of
fine particulate matter. Lignite, bituminous coal, and their blends with different
To further study the effects of coal blending on the char- blend ratios (9:1, 7:3, 5:5, 3:7 and 1:9) were combusted
acteristics of the particulate matter generated, the morphol- in a drop tube furnace under the O2/N2 and O2/CO2 atmos-
ogy of the particulate matter generated from coal blends pheres. The effects of coal blending on the formation and
combustion was examined. Figure 7 shows the morpholo- properties of particulate matter were studied. The mass size
gies of the particulates collected at the eleventh stage of LPI distribution, concentration, elemental composition and mor-
after coal blends combustion under O2/N2 atmosphere. The phology of the particulates generated were analyzed. The
particulates are generally spherical, usually formed from the results showed that:
minerals melted on the char surface [29]. Besides, because (1) Lignite XLT generated more PM1 and PM1-10 than bi-
of the interactions between the particulates generated from tuminous coal DT.
different formation mechanisms, a large number of small (2) The mineral interactions between the lignite and bi-
irregular-shaped particles were found on the surface of the tuminous coal suppressed the fine particulate generation
spherical particulates. The EDS result for the particle as during coal blends combustion.
marked in Figure 7 shows that the mole fraction of each (3) The blend ratio has significant impact on the suppres-
element in this particle is Al 11.1%, Si 8.3%, Ca 7.5%, Fe sion degree of the PM1 generation. In this experimental
21.4%, Mg 3.0% and O 48.7%, indicating that it is a mix- study, PM1 generation had a maximum suppression degree
ture of aluminosilicate and the elements Ca and Fe. It is at the blend ratio of 7:3.
further illustrated that, some of the volatile elements Ca and (4) The O2/CO2 atmosphere affected the formation and
ZHOU Ke, et al. Chinese Sci Bull October (2010) Vol.55 No.30 3455

Figure 7 Morphology of the particulates collected at the eleventh stage of LPI under O2/N2 combustion when the blend ratio is 7:3.

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