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助剂对Ni基催化剂结构及甲烷化性能的影响
引用本文:崔晓曦,孟凡会,何忠,李忠,郑华艳.助剂对Ni基催化剂结构及甲烷化性能的影响[J].无机化学学报,2014,30(2):277-283.
作者姓名:崔晓曦  孟凡会  何忠  李忠  郑华艳
作者单位:太原理工大学煤化工研究所, 煤科学与技术教育部和山西省重点实验室, 太原 030024;赛鼎工程有限公司, 太原 030032;太原理工大学煤化工研究所, 煤科学与技术教育部和山西省重点实验室, 太原 030024;太原理工大学煤化工研究所, 煤科学与技术教育部和山西省重点实验室, 太原 030024;太原理工大学煤化工研究所, 煤科学与技术教育部和山西省重点实验室, 太原 030024;太原理工大学煤化工研究所, 煤科学与技术教育部和山西省重点实验室, 太原 030024
基金项目:国家“973”计划(No.2012CB723105);山西省青年基金(No.2013021007-4);太原理工大学校青年基金(No.2012L040)资助项目。
摘    要:本文采用等体积浸渍制备了掺杂不同金属助剂改性的Ni基催化剂,考察了其催化浆态床CO甲烷化的性能。通过XRD、H2-TPR、HR-TEM等表征对催化剂进行了分析,结果表明,掺杂Zr、Co、Ce、Zn、La助剂促进了Ni物种在载体表面的分散,减小了Ni的晶粒尺寸,降低了催化剂的还原温度;掺杂Mg助剂则导致催化剂的还原温度升高。浆态床活性评价结果表明,掺杂Zr、Co、Ce、Zn、La助剂提高了催化剂的甲烷化性能,其中以La助剂的效果最明显,通过对La负载量进一步优化后发现,当La负载量为8%时,催化剂的甲烷化催化性能最优,CO转化率、CH4选择性和时空收率分别达到96.3%、87.1%和179.6 g·kg-1·h-1;掺杂Mg助剂则降低了催化剂的甲烷化活性。

关 键 词:浆态床反应器  CO甲烷化  Ni基催化剂  金属助剂
收稿时间:5/4/2013 12:00:00 AM
修稿时间:2013/7/26 0:00:00

Effects of Additives on Sturcture and Methanation Performance of Ni-Based Catalysts
CUI Xiao-Xi,MENG Fan-Hui,HE Zhong,LI Zhong and Zheng Hua-Yan.Effects of Additives on Sturcture and Methanation Performance of Ni-Based Catalysts[J].Chinese Journal of Inorganic Chemistry,2014,30(2):277-283.
Authors:CUI Xiao-Xi  MENG Fan-Hui  HE Zhong  LI Zhong and Zheng Hua-Yan
Institution:Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Sedin Engineering Company Limited, Taiyuan 030032, China;Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China;Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
Abstract:Nickel-based catalysts were prepared with different metal promoters by incipient impregnation method, and the catalytic performance of CO methanation were studied in slurry-bed reactor. XRD, H2-TPR, and HR-TEM were used to characterize the catalysts, the results show that additives of Zr, Co, Ce, Zn, La improved the dispersion of Nickel species on support, and decreased the particle size of Ni and reduced the reduction temperature of catalyst, while the additive of Mg increased the reduction temperature. The catalytic results show that additives of Zr, Co, Ce, Zn, La improved the catalytic performance of CO methanation in slurry-bed reactor, especially the catalyst with La additive. Further investigation shows that when the loading of La reached 8%, the catalyst exhibited the best catalytic performance, with the conversion of CO of 96.3%, the selectivity and space-time yield (STY) of CH4 of 87.1% and 179.6 g·kg-1·h-1, respectively. While the catalyst doped with Mg additivie decreased the catalytic performance.
Keywords:slurry-bed reactor  CO methanation  nickel-based catalyst  metal additives
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