文献类型：期刊文献

英文题名：Suppression of Methane Formation by Regulating the Hydrogenation Capability of Metal Oxides in Alkylation of Benzene with Syngas

作者：Zhao, Qichao[1];Zhao, Yitao[1];Zhuang, Jianguo[1];Zhang, Peng[1];Liu, Xinhui[1];Cheng, Junjun[1];Yu, Yijun[1];Wang, Yuchen[1];Liu, Zhen[2];Zhu, Xuedong[1];Yang, Fan[1]

机构：[1]East China Univ Sci & Technol, Engn Res Ctr Large Scale Reactor Engn & Technol, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China

年份：2022

卷号：61

期号：36

起止页码：13354

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20223812760663);WOS:【SCI-EXPANDED(收录号:WOS:000852030100001)】；

基金：? ACKNOWLEDGMENTS This project was sponsored financially by the National Natural Science Foundation of China (No. 21776076) and the Fundamental Research Funds for the Central Universities (JKA01211710) .

语种：英文

外文关键词：Alkylation - Benzene - Carbon monoxide - Catalyst activity - Cerium oxide - Density functional theory - Energy barriers - Hydrogenation - Metals - Synthesis gas - Zeolites

摘要：In alkylation of benzene with syngas, the inevitable converting of syngas into methane, as a side reaction, severely hinders the effective utilization of carbon monoxide (CO), which is a major challenge to circumvent. In this work, a series of bifunctional catalysts composed of various zinc/zirconium/cerium metal oxides and HZSM-5 zeolite were prepared in order to explore the key factor of methane formation and achieve high CO efficiency. The results show that methane selectivity mostly depends on the hydrogenation capability, which can be regulated via altering compositions of the metal oxides. Combined with density functional theory calculation and characterizations, it is found that the hydrogenation capability of metal oxide is related to the energy barrier of hydrogen (H-2) heterolysis. Compared to CeO2, the addition of zinc favors a lower energy barrier and a stronger ability toward H-2 heterolysis, while the addition of zirconium makes this ability weaker. Too strong heterolysis capability consequently leads to excessive hydrogenation, which further causes high methane selectivity; however, too weak heterolysis capability will lead to low catalytic activity. Hence, proper hydrogenation capability is an important element for low methane selectivity and high catalytic activity. Our findings reveal the formation mechanism of methane and provide a new strategy to reduce methane content.