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International Journal of Greenhouse Gas Control xx (2012) xxxxxx

Emission of NOx and N2 O from co-combustion of coal and biomasses in CFB combustor

Teerachai Saikaew, Prajak Supudommak, Lursuang Mekasut, Pornpote Piumsomboon, Prapan Kuchonthara Effect of biomass types on NO and N2 O emissions from co-combustion with coal was investigated in a CFB combustor. Nitrogen content in biomass feedstock was found to have more signicant effect than nitrogen in air on the NO and N2 O formation during co-combustion in the CFB. The emission of NO and N2 O in the CFB can be controlled by manipulating air injection along the riser.

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Emission of NOx and N2 O from co-combustion of coal and biomasses in CFB combustor
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Teerachai Saikaew a,b , Prajak Supudommak a,b , Lursuang Mekasut a,b , Pornpote Piumsomboon a,b , Prapan Kuchonthara a,b,
a b

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Fuels Research Center, Department of Chemical Technology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand Center of Excellence for Petroleum, Petrochemical and Advanced Materials, Chulalongkorn University, Bangkok 10330, Thailand

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a r t i c l e

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a b s t r a c t
Utilization of biomass in combustion processes is a promising way to reduce net emission of greenhouse gas, e.g. CO2 , to atmosphere. However, biomass is not likely to be successfully employed as a single feedstock due to its low energy density compared to coal. The co-combustion of coal and biomass in a circulating uidized bed combustor (CFBC) can be employed to address this issue by improving the overall caloric value. This work investigates the inuences of different biomass types on CFBC emissions. Subbituminous coal along with four biomass types such as palm shell, coconut shell, sawdust and rice husk were employed in study. The results indicated that the temperature prole in the riser was matter relevant to the heating value of fuel mixtures. The co-combustion of coal and palm shell gave the highest average combustion temperature, due to comparable heating value of both fuels. On the other hand, the cocombustion of coal and rice husk, which has relatively lower heating value, gave the lowest temperature. The presence of biomass in combustion was found to lead to a reduction of NOx and N2 O in ue gas. The fuel-nitrogen content was observed to be a major factor for determining both NOx and N2 O emission. Moreover, this work exhibited that the injection of secondary air with different position into the riser inuenced the NOx and N2 O concentration in the ue gas. 2012 Published by Elsevier Ltd.

Article history: Received 23 September 2010 Received in revised form 13 May 2012 Accepted 17 May 2012 Available online xxx Keywords: Coal Biomass Circulating uidized bed Combustion NOx N2 O

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1. Introduction The world energy demand has been continuously increasing due to the population growth and the improved living standards especially in developing countries such as China and India. Currently, most of the energy supplies are based on fossil fuel such as coal, oil and natural gas. Combustion is a typical chemical process utilized with these fuels in most energy production systems. The main byproduct from these processes is carbon dioxide which is the major contributor to the greenhouse gases. Thus, in order to reduce the carbon dioxide emission, the fuel types have to be changed. Biomasses, abundant resources in tropical countries, were considered as candidates. Since the carbon dioxide emitted from the biomass combustion is in the natural carbon cycle, it is generally assumed that the total amount of carbon dioxide in the atmosphere does not increase. With appropriate technology, biomass can partially substitute the fossil fuels. A circulating uidized bed combustor (CFBC) is a technology being widely employed for

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Corresponding author at: Fuels Research Center, Department of Chemical Technology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand. Tel.: +66 2 218 7519; fax: +66 2 255 5831. E-mail address: prapan.k@chula.ac.th (P. Kuchonthara). 1750-5836/$ see front matter 2012 Published by Elsevier Ltd. http://dx.doi.org/10.1016/j.ijggc.2012.05.014

combustion because of its abilities to handle various types of fuel such as coal, especially low-quality coals, biomass and wastes. The CFBC technology is also of great benet to the environment due to its high efciency and low emission characteristics (Kerr and Probert, 1986). Although the use of biomass is an effective approach too reduce the CO2 emissions, the release of other pollutants and greenhouse gases such as oxides of sulphur and nitrogen needs also to be investigated. Some of these gases are considerably more potent than CO2 . For example, the global warming potential (GWP) of N2 O is equivalent to 296 kgCO2 within a time horizon of 100 years (Tanaka et al., 2009). Therefore, there are a number of researchers who presented results of their study of the emission from CFBCs, especially the oxide of nitrogen. Amand and Leckner (1994) studied the reduction of N2 O in a CFBC. They concluded that the N2 O emission was mainly caused by the nitrogen in low volatile fuels during the combustion process. Reidick and Kremer (1996) showed that stoichiometric ratio of primary air and the residence time in the combustor section before the secondary air are of main importance to the pollutant formation. The N2 O concentration in the ue gas is mainly determined by the homogeneous N2 O reduction through hydrogen radicals and the heterogeneous N2 O formation from NO reduction on the char surface. The understanding of the process equilibrium between NOx formation and destruction reactions in

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T. Saikaew et al. / International Journal of Greenhouse Gas Control xxx (2012) xxxxxx Table 1 Proximate analyses of coal and biomasses. Weight % Coal Fixed carbon Volatile matter Moisture Ash 38.66 35.84 17.11 8.39 Palm shell 11.96 77.60 5.78 4.66 Coconut shell 21.13 67.79 9.76 1.32 Sawdust 11.14 79.14 5.90 3.82 Rice husk 18.21 57.48 8.18 16.13

the CFBC was investigated by Zhao et al. (1997) using various fuels such as anthracite, bituminous, lignite and petroleum coke. They found a correlation between NOx concentration and the oxygen and local char concentrations. Later on Li et al. (1998) presented review of mechanisms and kinetics of NO and N2 O reduction reaction with coal chars in FBC (uidized bed combustor). Their studies showed that the N2 O could be reduced on the char surface more than NO. Temperature is also an important parameter for NO and N2 O reduction reactions. de Diego et al. (1996) also studied the effects of operating parameters which are temperature, excess air factor, secondary/total air ratio, limestone addition and coal particle size on NOx and N2 O. The reduction of N2 O emissions by secondary fuel injection has been investigated by Liu and Gibbs (1998). Ethane or propane was injected and more than 70% of N2 O reduction was achieved. The same research group later on studied the effects of coal properties on NOx and N2 O formation in CFBC (Liu et al., 2001). Zhao et al. (2006, 2003) investigated the effect of minerals in coal on oxide of nitrogen. They found that iron promotes NO reduction with CO and alkali metal catalyzed NOchar reaction. Teixeira and Lora (2004) studied the NOx emission from bagasse boilers in Brazil. Xie et al. (2007) presented their study resulted of the emissions of SO2 , NO and N2 O in a bench scale CFBC. Armesto et al. (2003) studied the coal characteristics on the N2 O formation in a FBC. They concluded that the important contributor of N2 O formation was the oxidation of charN and the temperature prole in the combustor, which strongly inuences N2 O emission. Shimizu and Toyono (2007) investigated the NOx and N2 O emission during the co-combustion of coal and dried sewage sludge. Tourunen et al. (2009) showed that N2 O emission increases when the bed temperature decreases. On the contrary, the N2 O emission decreases when the oxygen concentration decreases. There have been a few works concerning emissions of NOx and N2 O during co-combustion of coal and CFBC, particularly with different operating condition. This paper focused on investigating effect of different types of biomass on the emissions from co-combustion with coal in a 30 kWth CFBC. Domestic biomasses including palm shell, coconut shell, sawdust and rice husk were employed. Moreover, NOx and N2 O emission from the combustor with different position of secondary air injection was studied.

at the position between sampling port one and two of the thermocouples. The gas could be sampled from the port number 10 located at the gas exit from the scrubber as shown in Fig. 1. Then gas was analyzed by ue gas analyzer (Madur model GA-40T plus) which could measure the concentrations of O2 , CO, SO2 , NO and H2 S. Then the analyzer will estimate the concentration of CO2 , NO2 , and NOx . Moreover, ue gas was sampled and stored in gas bags which are subjected to gas chromatography (Thermo Finigan) with TC detector for analyzing N2 O concentration. 2.2. Fuels The sub-bituminous coal from Indonesia and biomasses, including palm shell, coconut shell, sawdust and rice husk, were used as fuels in this study. Particle size of both fuels was sieved to smaller than 1.2 mm. The proximate and ultimate analyses were performed by standard procedures and heating values were also measured using a bomb calorimeter. Metal and mineral elements in fuels were analyzed using X-ray uorescence (XRF) technique. The mass ratios of coal and rice husk were varied from 100:0, 50:50 and 0:100, during the experiments. The total feed rate of seven kilograms per hour of fuels to the riser was controlled. 3. Results and discussion 3.1. Physical and chemical properties of coal and biomasses Table 1 shows the proximate analyses of coal and selected biomasses. One can observe that the volatile mater in the biomass was two times higher than that in coal. On the other hand, coal has a higher xed carbon and, in this study, a higher moisture content. Among the biomass types, rice husk is the source which has the highest ash content. The result of ultimate analyses is given in Table 2. It can be noticed that both coal and biomass contain comparable amount of carbon, hydrogen, and oxygen content. However, coal has higher nitrogen and sulfur contents than the biomass types studied in this work. The thermal and physical properties of coal, the investigated biomass types, and sand are reported in Table 3. It was found that the gross heating values of coal and palm shell were comparable resulting in values around 22 MJ/kg. The heating values of the others were 2530% lower than that of coal or palm shell. Table 4 shows the metal oxides in coal and the biomass. Some of these metal oxides, such as iron oxide, magnesium oxide, could increase the emission of NOx during combustion (Shimizu and Toyono, 2007), while other oxides such as calcium oxide or
Table 2 Ultimate analyses of coal and biomasses. Weight % (daf) Coal C H N O S 52.22 4.97 1.33 40.80 0.68 Palm shell 45.36 5.65 0.65 48.25 0.09 Coconut shell 45.95 5.76 0.04 48.23 0.02 Sawdust 46.07 5.47 0.19 47.63 0.01 Rice husk 48.05 7.27 0.18 44.50 0.00

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2. Experimental 2.1. Test rig The co-combustion of coal and biomass was carried out in a 30 kWth circulating uidized bed combustor (CFBC). The CFBC was composed of a riser (3.0 m height and 0.1 m i.d.) and downcomer (1.6 m height and 0.2 m i.d.) connecting through a L-valve (0.05 m i.d.), as shown in Fig. 1. Along the height of the riser, eight thermocouple ports were set up. The rst port was 10 cm above the air distributor plate and the others were 40 cm apart. At the top of the riser, the cyclone was connected in order to separate particles from gas stream. The particles were recycled to the downcomer, while the gas stream was fed to the second cyclone to further separate very ne particles. The gas stream from the second cyclone was sent to the water scrubber to cool ue gas and to remove particulates before exhausting to atmosphere. The primary air was preheated to 600 C during the start-up process and the preheating was maintained until the process reached steady-state condition. The primary air was fed through the gas distributor. Its velocity in the riser was varied from 2 to 3 m s1 , depending on temperature prole. The secondary air was introduced into the riser at 1.0 m above the distributor plate. Sand with particle sizes between 200 and 300 m was used as the bed material. The fuels, coal and rice husk were fed separately through screw feeders into the riser

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Fig. 1. Schematic diagram of the CFBC system.

Table 3 Thermal and physical properties of coal, biomasses and sand. Coal Gross heating values (kJ/kg) Bulk density (g/L) Size ( m) 22,195 900.28 <1200 Palm shell 22,517 Coconut shell 18,721 Sawdust 16,783 Rice husk 14,960 131.48 <1200 Sand 2100 200300

Table 4 Metal oxide analyses for coal and biomasses. Metal Oxides Fe2 O3 SiO2 Na2 O MgO Al2 O3 SO3 CaO P2 O5 K2 O Other Weight % (daf) Coal 16.59 26.04 8.52 1.50 12.50 18.78 9.17 0.28 1.64 4.98 Palm shell 11.36 22.48 1.64 7.18 2.64 1.60 34.97 6.80 7.43 3.90 Coconut shell 21.49 10.20 5.87 2.17 2.54 4.23 10.16 3.71 28.75 10.88 Sawdust 2.94 8.18 2.21 9.48 1.84 4.27 46.60 4.04 15.49 4.95 Rice husk 2.02 83.40 1.07 1.15 0.57 1.06 2.47 2.72 3.85 1.69

ferric oxide, could promote the decomposition of N2 O (Tourunen et al., 2009). One can notice that the content of calcium oxide in the biomass was much higher than that in the selected coal. 3.2. Effect of fuel mixtures on temperature proles along the riser Fig. 2 shows the temperature prole along the riser when only coal was used as fuel. The primary air was fed from the bottom of the bed through the air distributor with the rate of 200 liter per minute (L/m) and the secondary air was fed at the rate of 100 L/m at the position of 2 m above the distributor. It can be observed that the temperature was slightly constant at 930 C in this section 1 m along the riser starting from the air distributor. Then, it gradually decreases along the riser from 900 C to 600 C. At this position, the secondary air was injected to the riser and the temperature rises again to 700 C and later on decreases. However, the

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Fig. 2. Temperature prole along the riser when coal being the only fuel for 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

Fig. 4. Temperature prole along the riser when coal and coconut shell being the only fuels for 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

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temperature drops drastically when it approached the secondary air feeding position. The reason was that the secondary air feeding to the riser was not preheated. Moreover, the injection port was located closed to the thermocouple probe. Its temperature was much lower than the temperature in the riser. Fig. 3 shows the temperature proles along the riser when coal and palm shell were mixed in different ratios and used as fuel. The proles of different mixtures display the similar patterns as that of coal. The more fraction of palm shell in the mixture resulted in a litter higher average bed temperature. This is attributable to a slight higher heating value of palm shell in comparison with coal. The temperatures in the riser along 1 m above the distributor are more or less constant around 900 C. Except the case of 70% palm

shell mixture, its temperature was approximately 1000 C. The reason is that palm shell can be burnt much faster than coal since its volatile matter was much higher while its heating value was comparable to coal (see Table 1). Later on, the temperatures decline due to the oxygen depletion and due to the low temperature of secondary air feeding as mentioned in the previous paragraph. After the gas passes the secondary air feeding position, the temperatures start rising again due to further fuel combustions and eventually decline. The proles also show that the mixtures with higher content of palm shell gave slightly higher temperature in the riser. This is consistent with the heating value of this type of biomass which is somewhat higher than that of the coal. Fig. 4 shows the temperature proles along the riser when coal and coconut shell were mixed in different ratio and used as fuel. The proles of different mixtures mainly display the same patterns. Since the heating value of the coconut shell is less than coal by 15%, therefore, the temperature proles of the fuel mixtures with higher content of coconut shell gave lower temperature than that of the coal. The inuence of heating value of biomass was emphasized when coal was mixed with other low-heating value biomass types. Figs. 5 and 6 depict the temperature proles along the riser when coal with sawdust and with rice husk were mixed and used as fuels with different compositions. The temperature along the riser became lower with increasing the content of the biomasses. A considerable drop in temperature was observed in case of rice husk. This corresponds to the obviously low heating value of rice husk in comparison with that of coal. 3.3. Effect of fuel mixtures on NOx and N2 O proles along the riser The ue gas was sampled from the port number 10 which was located above the scrubber. Fig. 7 shows the NOx concentration in the ue gas from the combustion of various mixtures between coal and biomass with different biomasses. The presence of biomass in fuels reduces the NOx concentration in the ue gas, particularly in case of coconut shell. This is coincided with the nitrogen contents in each biomass as shown in Table 2. The lowest content of nitrogen in coconut shell explains why the fuel mixture of coal and coconut shell exhibited the lowest NOx concentration.

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Fig. 3. Temperature prole along the riser when coal and palm shell being the only fuels for 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

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Fig. 7. NOx concentration from the combustion of various mixtures between coal and biomass when using 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

Fig. 5. Temperature prole along the riser when coal and sawdust being the only fuels for 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.
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Fig. 8 shows the N2 O concentration in the ue gas. The N2 O concentration gradually decreases with the increment of the biomass content in the fuel mixture. The concentration value, to some degree, shows a linear relationship with the content of biomass in the mixture. The N2 O reduction indicates that the formation of N2 O is signicantly dependent on the fuel-nitrogen. In case of the mixture of coal and palm shell with the ratio of 70:30, the N2 O concentration becomes slightly higher in comparison with in case of coal alone. This is attributable to the relatively higher nitrogen content in palm shell than other biomass types. Additionally, the combustion of 70:30 coalpalm shell mixture gave higher temperature in the lower region of the riser as shown in Fig. 3. This condition enhanced the NO formation during the combustion at the lower

Fig. 8. N2 O concentration from the combustion of various mixtures between coal and biomass when using 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

part of the riser. Then this NO reacted with carbon in char in the upper region to produce N2 O and CO where the temperature was lower along the riser height (Basu, 2006; Winter et al., 1999). Fig. 8 also shows that the coalcoconut shell mixture provides the least N2 O emission corresponding to its lowest nitrogen content.

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Fig. 6. Temperature prole along the riser when coal and rice husk being the only fuels for 200 lpm of primary air and 100 lpm of secondary air at 2 m from the distributor.

Fig. 9. Temperature proles along the riser when the location of secondary air feed at 1, 2, and 2.4 m above the distributor.

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Fig. 12. N2 O concentration from the combustion of coal and the mixtures of coal and biomass at 50:50 when using 200 lpm of primary air and 100 lpm of secondary air at different location (1, 2, and 2.4 m).

Fig. 10. NOx and N2 O concentration when the location of secondary air feed at 1, 2, and 2.4 m above the distributor.

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3.4. Effect of the location of secondary air feeding Three locations of secondary air feeding were investigated. These are 1, 2, and 2.4 m from the distributor. Fig. 9 shows the temperature prole when only coal was used as the fuel with different locations of secondary air feeding. One can observe that when the feeding location was at 1 m, the average temperature along the riser was lower than that when the location at 2 and 2.4 m. The average temperatures along the riser, when the secondary air feeding location was at 2 and 2.4 m, were approximately the same. Fig. 10 shows the NOx and N2 O concentration at different locations of secondary air feeding. It shows that both NOx and N2 O concentration decreased when the location of secondary air moved upward from 1 to 2.4 m. An explanation for NOx was when the secondary air feeding was near the distributor, the secondary air provides excess oxygen to promote the fuel-nitrogen oxidation in the high temperature zone. On the other hand, when the secondary air feeding was located in the upper zone (2.4 m), the inuence of oxygen on the nitrogen oxidation was less since the temperature in the upper region was much lower than the lower region. Nitrous oxide, N2 O, concentration was found to be followed the same trend as NOx concentration. The explanation could be different. The N2 O would be produced from the reaction between NO and fuel-nitrogen. In case of secondary-air feeding at 1 m, large amount of NO could be produced and reacted with fuel-nitrogen due to the release of volatile

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matter. The NOx and N2 O concentrations from the combustion of various fuel mixtures were plotted in Figs. 11 and 12. The NOx and N2 O concentrations leaving the scrubber were very much the same independent on whether the secondary air feeding was located at 2 or 2.4 m, except the case of sawdust. The reason could be that sawdust contained high composition of CaO as shown in Table 2. There are a number of literature (Hou et al., 2008; Shimizu and Toyono, 2007) stated that CaO acts as catalyst for the reduction of nitrogen oxide especially in the region of excess oxygen. 4. Conclusion The effects of different biomass types on performance of cocombustion with coal in a circulating uidized bed combustor (CFBC) were investigated. The emission on NOx and N2 O was also examined during the co-combustion of coal and biomass with different blending ratios. The results indicated that the temperature prole in the riser is matter relevant to the heating value of fuel mixtures. Among different biomass types, palm shell has the highest caloric value, which is comparable to coal. Thus the co-combustion of coal and palm shell gives the highest average combustion temperature. On the other hand, the co-combustion of coal and rice husk gives the lowest temperature. The fuel-nitrogen content was found to be a major factor affecting NOx and N2 O emission. Co-combustion of coal and coconut shell, which has the lowest nitrogen content, gives an obviously low both NOx and N2 O emission, despite the comparable combustion temperature. Additionally, the change in injection position of the secondary air from 1 to 2.4 m could conne the oxygen concentration in the primary combustion zone, resulting in the further lower emissions of NOx and N2 O. References
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Fig. 11. NOx concentration from the combustion of coal and the mixtures of coal and biomass at 50:50 when using 200 lpm of primary air and 100 lpm of secondary air at different location (1, 2, and 2.4 m).

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Please cite this article in press as: Saikaew, T., et al., Emission of NOx and N2 O from co-combustion of coal and biomasses in CFB combustor. Int. J. Greenhouse Gas Control (2012), http://dx.doi.org/10.1016/j.ijggc.2012.05.014