文献类型：期刊文献

英文题名：Understanding kinetically interplaying reverse water-gas shift and Fischer-Tropsch synthesis during CO2 hydrogenation over Fe-based catalysts

作者：Xu, Minjie[1];Cao, Chenxi[1,2];Xu, Jing[1,3]

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

年份：2022

卷号：641

外文期刊名：APPLIED CATALYSIS A-GENERAL

收录：;EI(收录号：20222412212901);WOS:【SCI-EXPANDED(收录号:WOS:000833349900003)】；

基金：This work is supported by the National Natural Science Foundation of China (Basic Science Center Program 61988101), the National Natural Science Foundation of China (21878080 and 62073142), Fundamental Research Funds for the Central Universities (222202117006), and the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology.

语种：英文

外文关键词：CO2 hydrogenation; Iron-based catalyst; Alkali metal; Active sites; Intrinsic kinetics

摘要：Direct CO2 hydrogenation into linear alpha-olefins presents a promising route in carbon-neutral chemical manufacture. This work systematically investigated the variable interplay between Reverse Water-Gas Shift (RWGS) and Fischer-Tropsch Synthesis (FTS) during CO2 hydrogenation using model Na-Fe5C2 catalysts, combining dynamic/steady-state CO/CO2 hydrogenation performance, intrinsic kinetics and multiple characterization results. Na-Fe5C2 proves to be surface-enriched with FeOx sites over which RWGS readily proceeds. Meanwhile, CO2 conversion under integral reaction conditions is limited by the subsequent FTS step due to a lack of available FeCx sites. The catalyst performance is steered by the properties and relative quantities of the two different active sites. Na addition promotes the refresh of FeOx sites and beta-elimination of alkyl intermediates over FeCx sites, but at the cost of inhibiting the surface fraction of FeCx sites and thus the single-pass CO2 conversion. These fundamental understandings will enlighten further development of CO2 hydrogenation catalysts with improved hydrocarbon yields.