Cycle experiments on chemical looping combustion of coal using potassium-improved iron ore as oxygen carrier
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摘要: 对天然的铁矿石加以钾基修饰,在流化床上进行了煤化学链燃烧循环实验。研究了改性后的铁矿石对气体产物浓度及含碳气体体积分数影响的持续力。钾基铁矿石缩短了反应时间并明显提高了CO2浓度;在20次循环中,钾基铁矿石能明显提高CO2体积分数并降低CO体积分数,11次循环后,CO2体积分数稍有减少,CO体积分数略有增加。借助于扫描电镜与电子能谱(SEM-EDX)和X射线衍射(XRD),对不同循环后的载氧体进行表征。与纯铁矿石相比,前10次循环钾基铁矿石载氧体表面严重烧结,20次循环之后烧结减轻,恢复多孔结构。结果表明,钾基铁矿石载氧体中KFe11O17或其衍生物对煤气化有催化作用;在20次循环中存在钾流失现象;20次循环后钾基铁矿石载氧体能完全氧化为Fe2O3。Abstract: The cycle experiments on chemical looping combustion of coal were carried out in a fluidized bed using a K-promoted iron ore as oxygen carrier. The continued effect of the K-promoted iron ore on the gas compositions, fractions of carbonaceous gases was investigated.The results showed that the reaction time was shortened by the K-promoted iron ore,and that the CO2 concentration was significantly increased.The CO2 fraction for the K-promoted iron ore was much higher than that for the iron ore whereas,the CO fraction was much lower during 20 cycles.After 11 cycles, the CO2 fraction slightly decreased with a slight increase in CO fraction for the K-promoted iron ore. The reduced oxygen carriers after different cycles were characterized by SEM-EDS (Scanning Electron Microscope-Energy Dispersive Spectrometer) and XRD (X-ray diffraction).Compared with pure iron ore, the K-promoted iron ore showed serious sinter on the oxygen carrier particles during the first 11 cycles. The oxygen carrier, however, re-obtained the porous structure after 20 cycles due to the loss of potassium.The XRD showed that the KFe11O17 or its derivatives displayed the catalytic effect on coal gasification in the process of chemical looping combustion and the oxygen carrier could be regenerated to Fe2O3 after 20 cycles.
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Key words:
- potassium /
- iron ore /
- coal /
- chemical looping combustion
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RICHTER H, KNOCHE K.Reversibility of combustion processes[J]. ACS Symp Ser, 1983, 235:71-86. 金红光, 王宝群. 化学能梯级利用机理探讨[J]. 工程热物理学报, 2004, 25(2): 181-184. (JIN Hong-guang, WANG Bao-qun. Principle of cascading utilization of chemical energy[J]. Journal of Engineering Thermophysics, 2004, 25(2): 181-184.) De DIEGO L F, GARCíA-LABIANO F, ADÁNEZ J, GAYAN P, ABAD A, CORBELLA B M, PALACIOS J M. Development of Cu-based oxygen carriers for chemical-looping combustion[J]. Fuel, 2004, 83(13): 1749-1757. ABAD A, MATTISSON T, LYNGFELT A, JOHANSSON M. The use of iron oxide as oxygen carrier in a chemical-looping reactor[J]. Fuel, 2007, 86(7/8): 1021-1035. SHEN L, WU J, XIAO J. Experiment on chemical looping combustion of coal with NiO based oxygen carrier[J]. Combust Flame, 2009, 156(3): 721-728. CHO P, MATTISSON T, LYNGFELT A. Comparison of iron-, nickel-, copper-and manganese-based oxygen carriers for chemical-looping combustion[J]. Fuel, 2004, 83(9): 1215-1225. 郭庆杰, 田红景, 刘永卓. CaSO4的复合载氧体制备及其反应特性[J]. 太原理工大学学报, 2010, 41(5): 572-576. (GUO Qing-jie, TIAN Hong-jing, LIU Yong-zhuo. Preparation and reactivity behavior of compound CaSO4 oxygen carrier[J]. Journal of Taiyuan University of Technology, 2010, 41(5): 572-576.) 丁宁, 郑瑛, 罗聪, 吴琪珑, 傅培舫, 郑楚光. 化学链燃烧中CaSO4复合载氧体的实验研究[J]. 燃料化学学报, 2011, 39(3): 161-168. (DING Ning, ZHENG Ying, LUO Cong, WU Qi-long, FU Pei-fang, ZHENG Chu-guang. Investigation into compound CaSO4 oxygen carrier for chemical-looping combustion[J]. Journal of Fuel Chemistry and Technology, 2011, 39(3): 161-168. 王保文, 晏蓉, 郑瑛, 赵海波, 郑楚光. CaSO4氧载体煤基合成气化学链燃烧模拟研究[J]. 燃料化学学报, 2011, 39(4): 251-257. (WANG Bao-wen, YAN Rong, ZHENG Ying, ZHAO Hai-bo, ZHENG Chu-guang. Simulated investigation of chemical looping combustion with coal-derived syngas and CaSO4 oxygen carrier[J]. Journal of Fuel Chemistry and Technology, 2011, 39(4): 251-257.) 宋涛, 沈来宏, 肖军, 高正平, 顾海明, 张思文. 铁矿石载氧体化学链燃烧高温还原表征[J]. 燃料化学学报, 2011, 39(8): 567-574. (SONG Tao, SHEN Lai-hong, XIAO Jun, GAO Zheng-ping, GU Hai-ming, ZHANG Si-wen. Characterization of hematite oxygen carrier in chemical-looping combustion at a high reduction temperature[J]. Journal of Fuel Chemistry and Technology, 2011, 39(8): 567-574.) 高正平, 沈来宏, 肖军, 郑敏, 吴家桦. 煤化学链燃烧Fe2O3载氧体的反应性研究[J]. 燃料化学学报, 2009, 37(5): 513-520. (GAO Zheng-ping;SHEN Lai-hong;XIAO Jun;ZHENG Min;WU Jia-hua. Analysis of reactivity of Fe-based oxygen carrier with coal during chemical-looping combustion[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 513-520.) LEION H, LYNGFELT A, JOHANSSON M, JERNDAL E, MATTISSON T. The use of ilmenite as an oxygen carrier in chemical-looping combustion[J]. Chem Eng Res Des, 2008, 86(9): 1017-1026. BERGUERAND N, LYNGFELT A. The use of petroleum coke as fuel in a 10kWth chemical-looping combustor[J]. Int J Greenhouse Gas Control, 2008, 2(2): 169-179. ADANEZ J, CUADRAT A, ABAD A, GAYAN P, de DIEGO L F, GARCIA L F. Ilmenite activation during consecutive redox cycles in chemical-looping combustion[J]. Energy Fuels, 2010, 24(2): 1402-1413. 顾海明, 吴家桦, 郝建刚, 沈来宏, 肖军. 基于赤铁矿载氧体的串行流化床煤化学链燃烧试验[J]. 中国电机工程学报, 2010, 30(17): 51-56. (GU Hai-ming, WU Jia-hua, HAO Jian-gang, SHEN Lai-hong, XIAO Jun. Experiments on chemical looping combustion of coal in interconnected fluidized bed using hematite as oxygen carrier[J]. Proceedings of the CSEE, 2010, 30(17): 51-56.) CAO Y, PAN W-P. Investigation of chemical looping combustion by solid fuels: 1 Process analysis [J]. Energy Fuels, 2006, 20(5): 1836-1844. CAO Y, CASENAS B, PAN W-P. Investigation of chemical looping combustion by solid fuels: 2 Redox reaction kinetics and product characterization with coal, biomass, and solid waste as solid fuels and CuO as an oxygen carrier[J]. Energy Fuels, 2006, 20(5): 1845-1854. WOOD B J, SANCIER K M. The mechanism of the catalytic gasification of coal char: A critical review [J]. Catal Rev Sci Eng, 1984, 26(2): 233-279. SHETH A C, SASTRY C, YEBOAH Y D, XU Y, AGARWAL P. Catalytic gasification of coal using eutectic salts: Reaction kinetics for hydrogasification using binary and ternary eutectic catalysts [J]. Fuel, 2004, 83(4/5): 557-572. RADOVIC L R, WALKER J, PHILIP L, JENKINS R G. Catalytic coal gasification: Use of calcium versus potassium [J]. Fuel, 1984, 63(7): 1028-1030. McKEE D W, CHATTERJI D. The catalytic behavior of alkali metal carbonates and oxides in graphite oxidation reactions[J]. Carbon, 1975, 13(5): 381-390. HUANG Y, YIN X, WU C, WANG C, XIE J, ZHOU Z, MA L, LI H. Effects of metal catalysts on CO2 gasification reactivity of biomass char[J]. Biotechnol Adv, 2009, 27(5): 568-572.
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