Performance of Fe2O3/LaFeO3 as oxygen carrier in chemical-looping hydrogen generation
-
摘要: 采用柠檬酸络合法制备Fe2O3/LaFeO3复合氧化物,将该氧化物作为化学链制氢过程的载氧体,在反应温度为900 ℃、常压下,对Fe2O3/CH4(剂烷比)、进水量、金属负载量进行了考察。结果表明,剂烷比为2:1、进水量为0.1 mL、质量分数15%Fe时载氧体性能最好,甲烷转化率达到60%,单次循环氢气产量为45 mL。将该评价结果与XRD和H2-TPR表征结果进行关联发现,反应过程的活性位不是金属氧化物,而是吸附氧,而且吸附氧越容易还原,甲烷转化率和氢气产量越高。通过连续60次还原-氧化循环发现,该载氧体上甲烷转化率和氢气产量比较稳定,循环后仍然保持钙钛矿结构。Abstract: Fe2O3/LaFeO3 was prepared by citric acid complexation method and used as oxygen carrier in chemical-looping hydrogen generation; the effect of Fe2O3/CH4 ratio, stream amount and metal loading on the performance of Fe2O3/LaFeO3 as oxygen carrier at 900 ℃ and atmospheric pressure were investigated. The results showed that the oxygen carrier performs best with CH4 conversion of 60% and single-loop H2 output of 45 mL, when the ratio of Fe2O3/CH4, stream input and Fe loading are 2, 0.1 mL, 15%, respectively. The XRD and H2-TPR results suggest that the active site is the adsorbed oxygen rather than metal oxide; the easier for the reduction of the adsorbed oxygen, the higher are the conversion of CH4 and the output of H2. Moreover, the oxygen carrier is still in perovskite structure and CH4 conversion and H2 output remain stable even after 60 cycles.
-
王艳辉, 吴迪镛, 迟建. 氢能及制氢的应用技术现状及发展趋势[J]. 化工进展, 2001, 20(1): 6-8. (WANG Yan-hui, WU Di-yong, CHI Jian. The status and development current of hydrogen energy and its application technology[J]. Chemical Industry and Engineering Progress, 2001, 20(1): 6-8.) BARRETO L, MAKIHIRA A, RIAHI K. The hydrogen economy in the 21st century: A sustainable development scenario[J]. Int J Hydrogen Energy, 2003, 28(3): 267-284. 王金全, 王春明, 张永, 徐晔, 贾东升. 氢能发电及其应用前景[J]. 解放军理工大学学报(自然科学版), 2002, 3(6): 50-56. (WANG Jin-quan, WANG Chun-ming, ZHANG Yong, XU Ye, JIA Dong-sheng. Hydrogen-power and its prospects for applications[J]. Journal of Pla University of Science and Technology(Natural Science Edition), 2002, 3(6): 50-56.) 卢玲玲, 王树众, 姜峰, 胡昕. 化学链燃烧技术的研究现状及进展[J]. 现代化工, 2007, 27(8): 17-22. (LU Ling-ling, WANG Shu-zhong, JIANG Feng, HU Xin. Research status and advances in chemical-looping combustion[J]. Modern Chemical Industry, 2007, 27(8): 17-22.) FAN L H, LI F X, RAMKUMAR S. Utilization of chemical looping strategy in coal gasification processes[J]. Particuology, 2008, 6(3): 131-142. RYDEN M, LYNGFELT A. Using steam reforming to produce hydrogen with carbon dioxide capture by chemical-looping combustion[J]. Int J Hydrogen Energy, 2006, 31(10): 1271-1283. YANG J B, CAI N S, LI Z S. Hydrogen production from the steam-iron process with direct reduction of iron oxide by chemical looping combustion of coal char[J]. Energy Fuels, 2008, 22(4): 2570-2579. 向文国, 狄藤藤. Ni载体整体煤气化链式燃烧联合循环性能[J]. 化工学报, 2007, 58(7): 1816-1821. (XIANG Wen-guo, DI Teng-teng. Performance investigation of Ni-based CLC gasification combined cycle[J]. Journal of Chemical Industry and Engineering(China), 2007, 58(7): 1816-1821.) ADANEZ J, GARCIA-LABIANO F, DE DIEGO L F, GAYAN P, CELAYA J, ABAD A. Nickel-copper oxygen carriers to reach zero CO and H2 emissions in chemical-looping combustion[J]. Ind Eng Chem Res, 2006, 45: 2617-2625. 高正平, 沈来宏, 肖军. 基于NiO载氧体的煤化学链燃烧实验[J]. 化工学报, 2008, 59(5): 1242-1249. (GAO Zheng-ping, SHEN Lai-hong, XIAO Jun. Chemical looping combustion of coal based on NiO oxygen carrier[J]. Journal of Chemical Industry and Engineering(Chiina), 2008, 59(5): 1242-1249.) 段维慧, 张建民, 陈磊, 屈星星, 林浩. 化学链燃烧技术的研究现状[J]. 山西能源与节能, 2007, 44(1): 31-34. (DUAN Wei-hui, ZHANG Jian-min, CHEN Lei, QU Xing-xing, LIN Hao. Research status of chemical looping combustion technology[J]. ShanXi Energy and Conservation, 2007, 44(1): 31-34) 刘黎明, 赵海波, 郑楚光. 化学链燃烧方式中氧载体的研究进展[J]. 煤炭转化, 2006, 29(3): 83-92. (LIU Li-ming, ZHAO Hai-bo, ZHENG Chu-guang. Advance on oxygen carriers of chemical-looping combustion[J]. Coal Conversion, 2006, 29(3): 83-92.) BEDEL L, ROGER A C, ESTOURNED C, KIENNEMANN A.CoO from partial reduction of La(Co, Fe)O3 perovskites for Fischer-Tropsch synthesis[J]. Catal Today, 2003, 85(2/4): 207-218. 郭文锋, 徐庆, 陈文, 黄端平, 王皓, 袁润章. La0.8Ca0.2Cr0.3O3钙钛矿复合氧化物的GNP法合成与表征[J]. 稀有金属材料与工程, 2005, 34(12): 1886-1889. (GUO Wen-feng, XU Qing, CHEN Wen, HUANG Rui-ping, WANG Hao, YUAN Run-zhang. Characterization of perovskite-type composite oxides of La0.8Ca0.2Cr0.3O3 synthesized by the glycine-nitrate process[J]. Rare Metal Materials and Engineering, 2005, 34(12): 1886-1889.) 郑瑛, 边关, 罗聪, 吴琪珑, 郑楚光. 钙钛矿型复合载氧体的制备及释氧性能研究[J]. 中国电机工程学报, 2011, 31(35): 90-96. (ZHENG Ying, BIAN Guan, LUO Cong, WU Qi-long, ZHENG Chu-guang. Investigation on the preparation and oxygen desorption ability of different perovskite sorbents[J]. Proceedings of the CSEE, 2011, 31(35): 90-96.) 张慧敏, 胡瑞生, 胡佳楠, 张玉龙. La2CoAlO6催化剂的指标及其甲烷催化燃烧性能[J].物理化学学报, 2011, 27(5): 1169-1175. (ZHANG Hui-min, HU Rui-sheng, HU Jia-nan, ZHANG Yu-long. Preparation and catalytic activities of La2CoAlO6 for methane combustion[J]. Acta Physico-Chimica Sinica, 2011, 27(5): 1169-1175.) 代小平, 余长春. LaMO3纳米复合钙钛矿氧载体化学循环重整甲烷制合成气[J]. 催化学报, 2011, 32(8): 1411-1417. (DAI Xiao-ping, YU Chang-chun. Nano-perovskite-based (lamo3) oxygen carrier for syngas generation by chemical-looping reforming of methane[J]. Chinese Journal of Catalysis, 2011, 32(8): 1411-1417.)
点击查看大图
计量
- 文章访问数: 1174
- HTML全文浏览量: 42
- PDF下载量: 809
- 被引次数: 0