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Chemical Engineering Science 66 (2011) 2141–2148

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Reaction kinetics and producer gas compositions of steam gasification of coal and biomass blend chars, part 1: Experimental investigation
Qixiang Xu a, Shusheng Pang a,n, Tana Levi b
a b

Department of Chemical and Process Engineering, University of Canterbury, New Zealand CRL Energy Ltd., Wellington, New Zealand

a r t i c l e i n f o
Article history: Received 5 October 2010 Received in revised form 27 January 2011 Accepted 10 February 2011 Available online 20 February 2011 Keywords: Steam gasification Producer gas Coal and biomass blend Solid char Kinetics Char conversion rate

Biomass and coal are important solid fuels for generation of hydrogen-rich syngas from steam gasification. In this work, experiments were performed in a bench-scale gasifier to investigate the effect of coal-to-biomass ratio and the reaction kinetics for gasification of chars of biomass, coal and coal–biomass blends. In the gasification of these chars, steam was used as the gasification agent, while nitrogen was used as a gas carrier. The gasification temperature was controlled at 850, 900 and 950 1C. Gas produced was analysed using a micro-GC from which carbon conversion rate was also determined. From the experiments, it is found that the coal and biomass chars have different gasification characteristics and the overall reaction rate decreases with an increase in the ratio of coal–to-biomass. The microstructure of the coal char and biomass char was examined using scanning electronic microscopy (SEM), and it was found that the biomass char is more amorphous, whereas the coal char has larger pore size. The former enhances the intrinsic reaction rate and the latter influences the intra particle mass transportation. The difference in mass transfer of the gasification agent into the char particles between the two fuels is dominant in the char gasification. & 2011 Elsevier Ltd. All rights reserved.

1. Introduction Heavy use of fossil fuels by human beings has caused serious concerns relating to the shortage of future energy and the negative impacts on environment, due to the green house gas (CO2) emissions. Extensive studies have been conducted recently in order to find alternative and sustainable sources for future energy and fuels. Biomass, originating from crops and trees, has attracted increasing interest as the full cycle of biomass growing and energy utilisation is considered to be largely carbon neutral. However, due to low energy density and the scattered distribution of the biomass, handling and transportation costs are high and this has hindered the potential for biomass utilisation for energy and fuels (Collot et al., 1999; McKendry, 2002). In order to reduce the production costs, the biomass can be blended with a proportion of high density coal for energy production through gasification. Gasification is an effective and efficient method for converting solid carbonaceous matters to hydrogen-rich syngas, called producer gas. This gas can either be directly used for generation of power and heat or be further synthesized to produce liquid fuel and chemicals. Of the various types of gasification technologies, fluidized bed gasification has advantages of high heat and mass transfer rates,


Corresponding author. E-mail address: (S. Pang).

and uniform temperature distribution in the gasifier, therefore, it is widely used in large scale operations. The overall process of solid fuel gasification within the fluidized bed reactor can be divided into two main steps after the initial short drying: (1) fast pyrolysis of the raw materials and (2) subsequent gasification of resultant chars. The former is a short process generating solid char and volatile gases. The latter consists of a series of heterogeneous reactions of the chars with gasification agent (air, oxygen or steam), and reactions among reactant and resultant gases. The char gasification process is a much slower conversion process compared to the initial pyrolysis, thus it is dominant in the whole gasification process (Everson et al., 2006). Extensive studies on gasification of either pure coal or pure biomass have been found in the literature. However, limited studies are reported on co-gasification of blended biomass and coal, and there is an apparent lack of fundamental understanding of the interactive effect of coal and biomass during the co-gasification. Due to the differences in blending ratio and diversity in fuel (biomass and coal) properties, the mechanism of co-gasification of the blend is complicated and the effects of the blending ratio on the gasification process is still unclear (Franco et al., 2003; Pan et al., 2000; Pinto et al., 2003, 2007). Coal, particularly the low quality coal such as lignite, contains significant amount of metal elements, which have catalytic effect on the gasification process (Clemens et al., 1998). Co-gasification of the blended biomass and coal has great potential for an effective use of existing and renewable sources in the future (Kumabe et al., 2007).

0009-2509/$ - see front matter & 2011 Elsevier Ltd. All rights reserved. doi:10.1016/j.ces.2011.02.026

lignite and wood (Eucalyptus nitens) were selected as the test materials. The nitrogen flow rate was controlled at 600 mL/min. 900 and 950 1C). By testing the five blended coal-to-biomass ratios (0:100. The producer gas generated from the gasification process flowed out with the carrier gas (nitrogen) via the outlet at the reactor bottom. the two feeds were thoroughly mixed in batches with blending ratios of coal-to-biomass of 20:80. biomass and their chars are listed in Table 1. For each condition. and to investigate the effects of two fuel blending. In each run. This is undesirable since the difference in residence time of the two fuels will limit the robustness of cogasification operation. In order to investigate the effect of the vapour diffusion resistance within the char particle. the pellets of all batches were firstly placed in an oven at 900 1C for 7 min to generate solid chars. no significant interactions were detected for the blend chars of bituminous and chestnut.67 0. 2008).. Raw lignite Moisture (wt%) Ash (wt%) Volatile (wt%) Fixed carbon (wt%) Total carbon (wt%) Total hydrogen (wt%) Total nitrogen (wt%) 19. the effective exposed area is increased. 80:20 and 100:0) at three operation temperatures (850. Contrarily. Finally the vapour-free producer gas was continuously analysed using the Micro-GC from which the producer gas releasing rate and its composition were obtained. which consists of a nitrogen and water feeding system. 1. 50:50 and 80:20.. 1 g samples of the chars were loaded in the tube reactor.9 34. 2005. By the addition of biomass to coal.1 50. which will be presented in the subsequent paper (Xu et al.9 – – 2. pressure and char diameter. nitens is a fast growing plantation hardwood species. For the gasification experiments. They found that the char activity is negatively affected by temperature. coal and their blends. Czechowskia and Kidawaa (1991) studied the reactivity of Janina bituminous coal char generated at 900 1C and found that the morphological changes of chars during the steam gasification promotes the reactivity at an internal surface of the char pore structure.2142 Q. (2009) showed that the char reactivity of Australian mallee wood has positive relationship with particle size. From this work.8 12. biomass and a 50:50 blend were examined using an SEM. The results from this study will be used in development and validation of a mathematical model of the solid char gasification. once the set temperature was reached.8 5 81. and to quantify the effects of the biomass–coal ratio on the gasification process. the investigation by Asadullah et al. the microstructure and morphology of chars of coal.. 2009). and then passed through a water bath to remove water vapour in the gas. the two fuels are segregated in feeding and fluidisation. apparent char reactivity was found to be increased with total surface area.4 0. 2009). This char generation process completely removed the volatile components. The gas mixture of nitrogen and generated steam was then fed to the top of the tube reactor and the steam reacted with the solid char particles. As the objective is to investigate the char gasification process. including two replicates. due to the increase in the retention time of the intrinsic metal elements. The information generated from this work will be used in the subsequent work on development of a full scale gasifier model. Fermoso and his colleagues (Fermoso et al. but significant interactions were observed for the blend chars of bituminous and olive stones. residues of chestnut and olive stones. a gas cooler and an on-line gas analyser (Micro-GC). a tube reactor. Lignite is a typical low quality coal . 2008).1 91. Porosities of the biomass char and the coal char were determined in terms of the mean pore diameters based on the SEM images. and thus the coal and the biomass are gasified separately. and the blends of these three fuels. In the study on radiata pine char by Cetin et al. and then milled separately to a particle size under 450 mm. due to density difference between biomass and coal. the coal and the biomass were dried to about 10% moisture content. that has vast reserves in New Zealand and E. 2010) investigated the reactivity of chars derived from a bituminous coal. three tests. because the interaction between these two fuels and the effective internal mass transfer resistance can be significant in the large sized pellets (Paviet et al. the char particles were tested in a bench-scale gasifier as shown in Fig.57 0.6 MPa. 900 or 950 1C. / Chemical Engineering Science 66 (2011) 2141–2148 In current practice of co-gasification. Each of the mixtures. a steam generator. and the actual steam gasification reactivity was determined. The properties of lignite. During the experiment. 2004).. a total number of 15 experimental runs were carried out. Xu et al.7 3. as well as pure lignite and pure biomass. After this.5 5. and the blended char reactivity can be increased by adding biomass to the coal (Zhu et al. 2011). which was placed into an electrically heated oven. From the literature review. 50:50. Cousins and colleagues (Cousins et al. the coal and the biomass are fed into the gasifier after mixing. The temperature in the reaction zone during the experiment was held at either 850.. The difference in the char reactivity between the two fuels is attributed to the differences in their structures and properties as the biomass char generally has lower density and is structurally more amorphous (Klose and Wolki. were performed.6 3. a separate set of experiments Table 1 Relevant properties of lignite and Eucalyptus nitens wood and derived chars. This paper will present the experimental work in which the gasification characteristics (kinetics and gas composition) are investigated and the microstructural differences between the coal char and the biomass char are examined. Experimental: materials and procedure In the experiments.7 47. (2005). Mastsumoto et al.. 20:80. Sadhukhan et al. The choice of the pellet size was to match the size of pellets that are used in practical domestic burners. Before the experiments.9 – – Wood char 0.5 12.. the co-gasification of the blend is uniform although the gasification characteristics may differ from the intrinsic reactions of each fuel.1 4.9 41.55 Raw wood 5. In this case.03 Lignite char 0. one solution is to pre-mix and press the mixture into pellets before being fed to the gasifier. In order to ensure the biomass and the coal to bind together through the whole gasification process.2 4 92. The objectives of this study are to both experimentally and theoretically investigate the gasification reactivity of chars of biomass. intrinsic char reactivity as an important fuel property is generally higher for the biomass than for the coal (Kastanaki and Vamvuka. the solid chars were held by a porous quartz frit near the bottom of the vertical tube reactor.38 81. In each run. Gasification kinetics of coal and biomass chars have been experimentally studied in recent years. hence the intrinsic reactivity of the coal is enhanced (Lu et al.4 82. The cylindrical pellets were formed by placing the feed into a mould and applying a pressure of 1. 2006) studied the char reactivity of Daw Mill coal with carbon dioxide. were compressed into pellets of 6 mm diameter and 10 mm length. the water pump was started and the steam generator was turned on. however. 2002. In order to understand the difference in gasification performance between the coal and the biomass..

4. the composition and generation rate of the producer gas as a function of elapsed time have been determined from the continuous Micro-GC analysis. it is seen that the char gasification can be divided into three stages: initial heat-up and slow gas production stage. carbon monoxide (CO) and carbon dioxide (CO2). Fig. 2–6. the gas composition of a given gas species can also represent the gas production rate of the species as the carrier gas (N2) had a constant volumetric flow rate (600 mL/min). The first stage took about 3 min and the gas production reached the maxima by the end of this stage. 1. which will be used for further analysis. Char gasification characteristics For each experimental run. The results for an operation at 900 1C are shown in Figs. 2. / Chemical Engineering Science 66 (2011) 2141–2148 2143 T Nitrogen Water Steam generator & Preheater Exhaust GC Water bottle & dehumidizer Gas cooler Char Fig. high concentration of a gas component means high production rate of this gas component. 3.Q. Results and discussion 3. Therefore. 20:80. as average values for the three replicate runs. a fast gas production stage and a final falling-rate gas production stage. Experimental setup of the bench-scale gasifier system. 2–6 for coal-tobiomass ratios of 0:100 (pure biomass). which had much smaller diameters than the original char particles. Profile of producer gas generation rate from gasification of biomass chars at 900 1C. Profile of producer gas generation rate from gasification of chars with coal-to-biomass ratio of 20:80 at 900 1C. In the figures. the nitrogen content was not shown as it only acted as a carrier and was not involved in the gasification reactions. 80:20 and 100:0 (pure coal). was conducted using milled chars of coal and biomass. During this stage. Fig. The maximum H2 compositions (mol/mol) at the end of the first stage of gasification for the five different coal-to-biomass . 3. From the results presented in Figs. 2–6. respectively.1. 50:50. The gas components of the char gasification producer gas were hydrogen (H2). Fig. In Figs. the maximum values of gas production rate for different fuels were different. Profile of producer gas generation rate from gasification of chars with coal-to-biomass ratio of 50:50 at 900 1C. Xu et al.

while for the pure coal char. . Carbon consumption rate for steam gasification of chars of pure biomass. In Fig. 8. 5) and 29% (Fig. 3–5. In the second and third stages of the gasification. the coal-to-biomass ratio has significant effects on the gas production rate. The identical gasification characteristics between the blended char and the coal char can be attributed to a number of factors. The results for steam gasification at 900 1C are shown in Fig. Based on the gas production rate and gas composition from the char gasification. 25% (Fig.7:27. pure coal and blended biomass and coal with coal-to-biomass ratio of 50:50. the second and third stages are not distinguishable. the biomass lost more volatile components than coal. and the gasification rate underwent an exponential decay approaching zero towards the end of the gasification process. 27% (Fig. 8 shows experimental results on the percentage char yield compared to the fresh fuel mass before the char generation. ratio chars were. Xu et al. Effect of blending ratio on char yield in the pyrolysis of char forming. thus the actual char mass formed from the biomass was less than that from the coal. respectively. 7. The maximum gas compositions for H2 and CO2 at the end of the first stage were much higher than those in the gasification of pure coal chars. 7 for chars of pure biomass. In Fig. It is interesting to note that once coal was added into the biomass to form a blend. the gas composition profile was significantly changed from the pure biomass (Fig. and then decreased towards zero in the third stage when the char conversion was completed. 2. In addition. / Chemical Engineering Science 66 (2011) 2141–2148 Fig. 6).3 in the blend char. 5. Therefore. 2) although only 20% coal was added. 35% (Fig. both the gas production rate and the trends were significantly different for chars with different coal-to-biomass ratios. the microstructures between the pure biomass and coal are different. the 50:50 coalto-biomass blend would be changed to the ratio of coal char-tobiomass char of 72. It can then be speculated that in the char generation of blended coal and biomass pellets. curves of gas production rate and composition for blended char are more identical to the pure coal gasification as shown in Figs. 3. after the initial heating up period. In other words. 36% (Fig. a higher proportion of the biomass was lost compared to the coal. 6). for the gasification of pure coal (Fig. In contrast. 2). CO and CO2) from the gas analysis. 3). 4). Fig. Fig. Profile of producer gas generation rate from gasification of coal chars at 900 1C. the solid carbon conversion rate can be determined as the solid chars are only converted to the three gases (H2. pure coals and blended coal and biomass at the blending ratio of 50:50. and thus the total gasification time was also different.2144 Q. Fig. The carbon conversion rate profile of blended char was similar to that of the pure coal char. and the coal becomes more influential than the biomass when being blended together. and hence the gasification characteristics. Profile of producer gas generation rate from gasification of chars with coal-to-biomass ratio of 80:20 at 900 1C. Fig. thus leaving more space for the coal char to cover. The carbon conversion rate can be used for further investigation of the gasification performance of various blending ratios of coal and biomass. In the char generation process before gasification. 6. the producer gas composition curves maintained a relatively constant rate for about 10 min in the second stage after reaching the maximum value. the carbon conversion rate continued decreasing after reaching the maximum value in the initial heating up period. It can be seen that the pure biomass char conversion rate maintained at a relative constant rate. followed by a falling rate. This will be discussed later in this paper. The char yield was only 15% for the pure biomass and this was increased linearly to 40% for the pure coal. for the gasification of pure biomass char.

after this point (0. which contain carbon (CO and CO2) in this study   vCO þ vCO2 PVN2 dC ¼ ð4Þ À dt vN2 RT where vCO. ÀdC=dt is the solid carbon consumption molar rate. the reactivity of pure biomass char increased rapidly and became the highest towards the end of the gasification. it Fig. The remaining carbon mass (m) at the given time can be determined as the difference between the initial total carbon mass and the accumulated carbon in the gases generated from the char gasification  Z t  dC m ¼ m0 À MWc dt À ð3Þ dt t¼0 In which MWC is the molar mass of the carbon in the gases generated from the char gasification (12 g/mol). it is concluded that adding coal-to-biomass has a negative effect on the gasification reactivity. In the meantime. Xu et al. the gasification reactivity for the coal char tended to be the lowest. Apparent gasification reactivity as a function of char conversion rate at 900 1C. Fig. 900 and 950 1C.4. respectively. 10. the molar consumption rate of solid carbon (ÀdC=dt) at any given time can be calculated by summating the molar flow rate of all gaseous species. had similar reactivity from the start until the char conversion reached 0. Fig. when the char conversion was completed and the results are shown in Fig. . or near the lowest. VN2 is the volumetric flow rate of nitrogen feed. The biomass char reactivity tended to be lower initially with a clear difference for gasification test at 950 1C. P and T are the pressure and temperature of nitrogen at the feed point.Q. 9–11 for gasification tests at 850. can be seen that all of the chars. Since the flow rate of an N2 feed was maintained constant through the experiment. the elapsed time for complete conversion of the chars was reduced.4 char conversion). vCO2 and vN2 are the instantaneous volumetric percentage of CO. / Chemical Engineering Science 66 (2011) 2141–2148 2145 3. which is defined as r¼À 1 dm 1 dX ¼ m dt 1ÀX dt ð1Þ where X is the conversion ratio of converted carbon to the initial total carbon mass (m0) during the gasification. The influence of gasification temperature can be due to the reduced difference in apparent activation energy between biomass and coal chars at higher temperatures. Fig.2. 12. From these figures. although the effect is reduced with increasing the gasification temperature. The results clearly demonstrate that with higher temperatures. therefore. except for the pure biomass chars. The results of the gasification reactivity for chars with various coal-to-biomass ratios are shown in Figs. Effect of blending on apparent char reactivity The apparent gasification reactivity of the char quantifies char conversion per unit time relative to the remaining carbon mass (m) at the given time (t). The influence of gasification temperature has been examined by comparing the elapsed time. 12 also shows that the complete carbon conversion time increased with the coal proportion in the blended chars. However. the molar flow rate of each gaseous species can be obtained from the instantaneous GC data. which can be determined from the GC gas analysis results. Apparent gasification reactivity as a function of char conversion rate at 850 1C. which is consistent with the reactivity analysis. 11. 600 mL/min in this case. whereas the reactivity of the blended chars fell between these two extreme cases. 9. thus the gasification reactivity was increased. CO2 and N2 in the producer gas mixture. Based on these findings. Apparent gasification reactivity as a function of char conversion rate at 950 1C. which is determined by X ¼ 1À m m0 ð2Þ The initial total carbon mass in the char (m0) was obtained as the mass difference between the char being loaded into the reactor and the ash remaining after the gasification test.

For the coal char. the char particle size was large enough to generate significant diffusion resistance that has competing effect with heterogeneous reactions. the resistance for the gas diffusion through the compact clusters plays a dominant role. These differences can be used to explain the different gasification characteristics between the biomass char and the coal char. and the effective reaction volume of the biomass char can be limited by the vapour diffusion resistance. because the vapour can penetrate into the char particle through the large cracks. (2) heterogeneous reaction on the surface of the char micro-pores and (3) gaseous products move out from the particles by diffusion under gas concentration gradient within the particle and by bulk gas flow. the carbonaceous materials are more likely to be segregated in the form of more compacted clusters and large cracks. On the other hand. For the biomass char. Therefore. . The results of comparison between pellet char and pulverised chars are shown in Fig. 13 from which it can be seen that in micrometre scale. However. the gasification reactions between the water vapour and the solid char occur within the whole volume of the char particle. The microstructure of the blended char shows the major characteristics of the coal char. the compacted clusters mean high resistance for the gas transfer from the compacted clusters to the large cracks.2146 Q. where large cracks and compacts clusters are observed. The electronic microscopic scanning images of surface of (a) pure biomass char. the vapour concentration within the particle is uniform and the whole solid volume would have similar conversion rate. For the biomass char. Fig. 13c). In the non-catalytic gas solid reactions between the steam and the solid char. 3. 15 for char conversion rate (X). For the coal char. the vapour molecules will initially react near the particle surface before they further diffuse into the centre of the solid particle. experiments were conducted using finer char particles of biomass and coal. 12. Xu et al. Analysis of char gasification mechanism During the char gasification using steam as the gasification agent. there are a large amount of finer voids between the carbonaceous matters forming the structure of thinner clusters. the coal char gasification exhibited typical first order reaction kinetics from which exponential decay in the reaction rate was observed. the fine voids can allow more uniform gas transfer through the gasification process. 14 for carbon consumption rate and in Fig. On the contrary as shown in Fig. In this study. All images have a magnification of  350. 2. In this case. / Chemical Engineering Science 66 (2011) 2141–2148 3. The resistance of inward diffusion of water vapour molecules into the char particles can be significant for the apparent char size of greater than millimetre level (Paviet et al.. it has been noticed that the overall gasification rate of biomass char maintained relatively constant after the initial heat-up period. thus high gasification reactivity can be maintained and increased with the elapsed time. if both the vapour diffusion resistance and intrinsic reaction rate are high enough. In this case. the overall reaction rate will be similar to the intrinsic reaction (Gupta and Saha. The observed differences in the char microstructures are consistent with previous findings of gas production and carbon conversion rates during the gasification process of these chars. 6. In order to verify the above hypothesis for the char gasification mechanism. which indicates an inhomogeneous reaction rate during the gasification. (b) 50:50 blended char and (c) pure coal char.4. 13. 13a) is significantly more amorphous than the coal char (Fig. This confirms that vapour diffusion resistance within the coal char can be negligible in the gasification compared to the intrinsic reaction rate. Therefore reactions occurred at and near the char particle surface. From Fig. 2008). 2003). Effect of gasification temperature and blending ratio on complete conversion time of the solid chars. Fig. if the vapour diffusion rate is significantly faster comparing with intrinsic reaction rate. due to gradient of partial pressure. there are three distinct steps which influence the overall gas production and carbon conversion rates: (1) diffusion of the steam molecules into the char particles.3. while the surface continuously moved inward with the char conversion. thus the diffusion of resultant gases is dominant. the biomass char matrix (Fig. the large cracks make it possible for fast gas transfer in the early stages of the gasification. Morphology of the chars The SEM images are illustrated in Fig.

the carbon consumption rate and the overall char conversion rate were only increased slightly after being milled to finer particles with smaller diameters. The difference in the vapour diffusion resistance between the biomass char and the coal char can be attributed to the distinct structural properties of these two solids. and this is followed by a falling rate in the last period of the process. However. Fig. In the initial heat-up stage. it is observed that for the coal char. Xu et al. a mathematical model has been developed to simulate the gasification process of biomass char. for the biomass chars. From the SEM analysis. On the other hand. Based on the above mechanisms. 2011). Effect of particle size on the char conversion rate: (a) biomass char and (b) coal char. The composition of the producer gas and gas production rate was continuously analysed by using a Micro-GC. hence the specific effective surface area is larger and the intrinsic reactivity is enhanced. which vary with the coal-to-biomass ratio. Effect of particle size on the carbon consumption rate: (a) biomass char and (b) coal char. which limits the inward diffusion of water vapour. coal char and blended biomass and coal char. This will be presented in the subsequent paper (Xu et al. carbon conversion rate and gasification reactivity were determined. coal chars and the chars of blended biomass and coal can be represented by three stages: initial heat-up and slow gasification stage. 14. the reaction rate decreases continuously after the maximum value is reached. fast gasification rate stage and falling rate stage. thus the particle diameter is not a critical factor. (2) The overall reactivity of the blended coal–biomass char decreases with the incremental fraction of the coal in the From these figures. A series of gasification tests were carried out in a benchscale gasifier at three different temperatures. 4. the biomass char is much more amorphous than the coal char. 15. From the study. the following conclusions are drawn: (1) The gasification of biomass chars.. carbon conversion rate and reactivity for gasification of biomass char.Q. the particle diameter was significantly reduced. the gasification rate increases to the maximum values. enhancing the carbon conversion rate significantly in the first and second stages of the gasification. Based on the gas analysis results. For gasification of the coal char. Conclusions Gas production rate. . This confirms that the vapour can easily diffuse into the coal char particles. However. the carbon conversion rate and overall char conversion rate of the milled chars were increased significantly compared to the original biomass pellet chars. In the milled biomass char particles. coal char and blended coal and biomass chars have been experimentally investigated in this work. which result in a larger effective pore diameter. The overall conversion rate of biomass char maintains at a relatively constant rate after the initial heat-up period. nitens and their blends at three different blending ratios. The reaction rate of the blended coal and biomass chars has intermediate characteristics with the trend similar to the coal char gasification. E. thus the surface area to the particle mass was much higher. The model is validated using the experimental results. the coal char shows denser cluster and large cracks. This is because the biomass loses more mass during the char generation. the diffusion rate is relatively slower due to the smaller pore size. / Chemical Engineering Science 66 (2011) 2141–2148 2147 Fig. The sample char particles were produced from the pellets of coal (lignite).

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