文献类型：期刊文献

英文题名：Ternary Fe-Zn-Al Spinel Catalyst for CO2 Hydrogenation to Linear α-Olefins: Synergy Effects between Al and Zn

作者：Xu, Minjie[1];Liu, Xianglin[1];Cao, Chenxi[1,3];Sun, Yang[1];Zhang, Chao[1];Yang, Zixu[1];Zhu, Minghui[1];Ding, Xiaoxu[1];Liu, Yitao[1];Tong, Zhangfa[2];Xu, Jing[1,2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]Guangxi Univ, Guangxi Key Lab Petrochem Resource Proc & Proc In, Sch Chem & Chem Engn, Nanning 530004, Peoples R China;[3]East China Univ Sci & Technol, Minist Educ, Key Lab Smart Mfg Energy Chem Proc, Shanghai 200237, Peoples R China

年份：2021

卷号：9

期号：41

起止页码：13818

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20214311080209);WOS:【SCI-EXPANDED(收录号:WOS:000710271700013)】；

基金：The National Natural Science Foundation of China (21878080, 21808058, and 61725301), Shanghai Sailing Program (18YF1406100), the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, International (Regional) Cooperation and Exchange Project (61720106008), and Fundamental Research Funds for the Central Universities (222202117006) are greatly acknowledged for funding this work. C.C. thanks the startup grant of East China University of Science and Technology (SLH00212012).

语种：英文

外文关键词：CO2 hydrogenation; linear alpha-olefins; Fe5C2; multiple additives; ternary Fe-Zn-Al spinel; synergy effect

摘要：Direct conversion of CO2 into linear alpha-olefins with Fe-based catalysts is promising both technically and economically. Al as a widely employed structural additive to Fe-based CO/CO2 hydrogenation catalysts is known to exhibit a side effect of shifting the selectivity from olefins to undesirable methane. Here, we report that by doping Zn into a binary Fe-Al spinel, a ternary Fe-Zn-Al spinel catalyst could be obtained with a high space-time yield with respect to linear alpha-olefins of 150.8 mmol(C).g(Fe)(-1).h(-1) in CO2 hydrogenation reactions. Multiple in situ/ex situ characterizations combined with DFT calculations illustrate that active Fe5C2 nanoparticles are wrapped with Fe-Al spinel overlayers with the introduction of Al alone, which is responsible for facilitating hydrogenation and inhibiting C-C coupling over the Fe-Al catalysts. Extra doping of Zn allows redistribution of Al to alleviate undesirable strong interactions between Fe5C2 and spinel phases, rendering a high selectivity to higher olefins. The revelation of a subtle synergy effect between Al and Zn underscores the pivotal role of precise tuning of multiple catalyst additives in optimizing the overall catalytic performance.