逆水煤气变换耦合乙烷脱氢反应中载体对氧化铬催化剂性能的影响

doi:10.16085/j.issn.1000-6613.2015.08.021

化工进展 ›› 2015, Vol. 34 ›› Issue (08): 3040-3043,3053.DOI: 10.16085/j.issn.1000-6613.2015.08.021

逆水煤气变换耦合乙烷脱氢反应中载体对氧化铬催化剂性能的影响

葛欣

南京大学化学化工学院, 江苏南京 210093

收稿日期:2014-10-30 修回日期:2014-12-20 出版日期:2015-08-05 发布日期:2015-08-05
作者简介:葛欣(1962—),男,博士,教授,研究方向为吸附与多相催化。E-mail xinge@nju.edu.cn。
基金资助:
基金项目:国家自然科学基金项目(21275069)。

Effect of supports on the catalytic performance of chromium oxide catalysts for the coupling of reversed water-gas shift reaction with the dehydrogenation of ethane to ethylene

GE Xin

School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China

Received:2014-10-30 Revised:2014-12-20 Online:2015-08-05 Published:2015-08-05

摘要/Abstract

摘要： 研究了在逆水煤气变换耦合乙烷脱氢反应中担载型氧化铬催化剂的活性,考察了多种载体对于催化剂反应性能的影响。结果表明,不同的载体所担载的氧化铬催化剂具有不同的催化性能。其中二氧化硅担载的氧化铬催化剂具有较高的乙烷转化率和乙烯选择性,在700℃时分别达到30.7%和96.5%。CO₂的作用是通过与H₂反应促进乙烷脱氢、并减少催化剂表面积炭。运用XRD、TPR、 XPS、UV-DRS和微量吸附量热技术对催化剂体相与表面结构、表面酸性和铬物种价态等进行了表征,结果显示催化剂表面酸中心适当的强度、数量和分布有利于乙烷的活化和催化转化,Cr³⁺和Cr⁶⁺物种是反应的活性中心。

关键词: 乙烷脱氢, 乙烯, 二氧化碳, 氧化铬, 催化剂载体

Abstract: The coupling reaction of the dehydrogenation of ethane to ethylene with reversed water-gas shift reaction was studied over chromium oxide catalysts. And the effect of support on catalytic activity was also studied. The results show that the support exerts a quite different effect on catalytic behavior. Cr/SiO₂ catalyst exhibits an excellent performance in this reaction with 30.7% ethane conversion and 96.5% ethylene selectivity. The function of CO₂ is to abstract H₂ and to resistant coke formation during dehydrogenation of ethane. XRD, TPR, XPS, UV-DRS spectroscopy and micro-calorimeter technique are used to investigate the nature of active site of catalysts. Characterization indicates that the distribution of chromium oxide on supports and surface chromium species structure are influenced by the nature of supports. The acidity/basicity and redox property of catalysts determines the catalytic activity in the dehydrogenation of ethane under CO₂. Cr³⁺and Cr⁶⁺ species on the surface of catalysts were proposed to be the active sites for the reaction.

Key words: ethane dehydrogenation, ethylene, carbon dioxide, chromium oxide, catalyst support

中图分类号:

葛欣. 逆水煤气变换耦合乙烷脱氢反应中载体对氧化铬催化剂性能的影响[J]. 化工进展, 2015, 34(08): 3040-3043,3053.

GE Xin. Effect of supports on the catalytic performance of chromium oxide catalysts for the coupling of reversed water-gas shift reaction with the dehydrogenation of ethane to ethylene[J]. Chemical Industry and Engineering Progree, 2015, 34(08): 3040-3043,3053.

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逆水煤气变换耦合乙烷脱氢反应中载体对氧化铬催化剂性能的影响

Effect of supports on the catalytic performance of chromium oxide catalysts for the coupling of reversed water-gas shift reaction with the dehydrogenation of ethane to ethylene

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