文献类型：期刊文献

英文题名：Synergistic Catalysis over Pd-Fe-Zn with Triple-Interface Structures for Selective CO2 Hydrogenation to Ethanol

作者：Ma, Yuling[1];Pu, Xin[2];Liu, Yangqin[1];Zhou, Peng[1];Han, Xin[3];Ye, Lei[1];Qin, Xinglong[1];Xu, Haitao[1];Kong, Lingtao[2];Li, Jiangbing[2];Zhang, Jian[4];Liu, Jichang[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Shihezi Univ, Sch Chem & Chem Engn, Shihezi 832003, Xinjiang, Peoples R China;[3]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai 200237, Peoples R China;[4]Xinjiang Jiayuheng Energy Technol Co LTD, Huyanghe 834034, Xinjiang, Peoples R China

年份：2025

卷号：15

期号：21

起止页码：18580

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20254419418396);WOS:【SCI-EXPANDED(收录号:WOS:001603543100001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (U22B20141, 22578281, 22508121, and 22408107), the Shanghai Sailing Program of China (23YF1409200), the China Postdoctoral Science Foundation (GZC20230800), the High-level Talents Launching Project from Shihezi University (RCZK202424), and the Tianchi Talent Program (Young Doctoral Program) of 2024 (CZ002731).

语种：英文

外文关键词：CO2 hydrogenation; ethanol; PdFe-basedcatalyst; C1 intermediate; synergistic catalysis

摘要：The hydrogenation of CO2 to ethanol is considered a promising route for recycling carbon resources while mitigating global warming. Nevertheless, the key scientific challenge lies in the efficient coordination of CO2 adsorption/activation, intermediate CO stabilization/dissociation, and selective C-C coupling within multistep cascade catalytic processes. Herein, we present a PdFe/NaZnOx catalyst with spatially coupled active centers to enhance cascade catalysis. Systematic characterization and DFT calculations reveal that the catalyst features a dynamic triple-interface structure driven by synergistic interactions among Pd, Fe3O4, and ZnO. This unique configuration achieves efficient CO2 hydrogenation to ethanol with a space-time yield of 87.5 mgg(cat)(-1)h(-1). Mechanistic insights demonstrate that Na-modified ZnO contributes the primary CO2 adsorption sites (0.125 mmol/g), while Pd synergizes with Fe3O4 to stabilize H-2 and intermediate CO, exhibiting a 4.1-fold enhancement in nondissociative CO activation compared to Fe/NaZnOx. Crucially, Pd facilitates in situ carburization of Fe3O4 to Fe5C2 (from 46.7 to 74.3%), forming Pd-Fe5C2 interfaces that drive *CO-*CHx coupling. The triple-interface structure enables the efficient transfer of *H/*CO intermediates, achieving 20.2% ethanol selectivity, which is 3.8 times higher than that of conventional Fe/NaZnOx. This work highlights the critical role of interfacial and metal-metal oxide synergy in optimizing C1 intermediate stabilization and cascade catalysis, providing a design strategy for multifunctional composite catalytic systems targeting hydrogenation of CO2 to ethanol.