文献类型：期刊文献

英文题名：Efficient Hydrogenation of CO2 to Higher Alcohols over Cu-Zn-Fe Catalysts: The Role of ZnFe2O4 Spinel Precursor

作者：Ma, Yuling[1];Liu, Shuang[1];Han, Xin[2];Ye, Lei[1];Xu, Haitao[1];Kong, Lingtao[3];Li, Jiangbing[3];Pu, Xin[3];Liu, Jichang[1,3]

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]East China Univ Sci & Technol, Sch Mech & Power Engn, Shanghai, Peoples R China;[3]Shihezi Univ, Sch Chem & Chem Engn, Shihezi 832003, Xinjiang, Peoples R China

年份：2026

卷号：14

期号：3

起止页码：1467

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20260419964776);WOS:【SCI-EXPANDED(收录号:WOS:001659667200001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (U22B20141, 22578281, and 22508121), the Shanghai Sailing Program of China (23YF1409200), 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; higher alcohol; CuFe-based catalyst; ZnFe2O4 spinel; C1 intermediate

摘要：Spinel-structured metal oxides offer unique advantages in heterogeneous catalysis due to their structural stability, tunable electronic properties, and multimetal synergistic effects. Herein, we strategically integrated ZnFe2O4 spinel with a conventional CuFe-based catalyst (CuFeOx) to enhance the catalytic performance for CO2 hydrogenation to higher alcohols, achieving a higher alcohol selectivity of 28.9% over the CuZnFeOx catalyst. In the catalyst, ZnFe2O4 stably anchors CuO via strong interfacial adhesion (3.3 J/m(2)) to form a stable CuO-ZnFe2O4 interface structure that promotes Cu dispersion. And during the subsequent reduction process, this structure modulates the reducibility of Fe3+ via Cu-ZnFe2O4 synergy, thereby facilitating in situ formation of FeCx sites (FeCx content, 51.6 -> 67.7%) in the reaction. Mechanistically, the precisely tuned Cu and FeCx dual-active centers effectively optimize the nondissociative and dissociative activation of CO, promoting C-C coupling for higher alcohol synthesis. Furthermore, oxygen-vacancy-rich ZnO provides additional CO2 adsorption sites (-1.46 eV) and synergistically stabilizes H-2/CO species at Cu/Fe active centers. Ultimately, the CO2 conversion on the CuZnFeOx catalyst increases to 35.2%, and the space-time yield for higher alcohols reaches 125.1 mgg(cat)(-1)h(-1), which is 4.4 times higher than that of the CuFeOx catalyst. This study establishes a catalyst design strategy that utilizes ZnFe2O4 spinel integration to regulate the final active structure for the optimized catalytic performance.