文献类型：期刊文献

英文题名：Concurrently Maximize CO2RR and Minimize HER: A Dual Catalytic Active Site Approach for Ampere-Level CO2-to-CO Electrolysis

作者：Fu, Huai Qin[1];Zhou, Min[2,3];Yu, Tingting[4];Yang, Yuwei[5];Sun, Ji Wei[6];Bedford, Nicholas M.[5];Wang, Liang[1];Liu, Porun[1];Lian, Cheng[7];Wang, Haifeng[2,3];Yang, Hua Gui[6];Zhao, Huijun[1]

机构：[1]Griffith Univ, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[2]East China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[5]Univ New South Wales, Sch Chem Engn, Sydney, NSW 2052, Australia;[6]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[7]East China Univ Sci & Technol, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2026

卷号：65

期号：6

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20260119842705);WOS:【SCI-EXPANDED(收录号:WOS:001648575000001)】；

基金：This work was financially supported by National Key Research and Development Program of China (2021YFA1500700), Australian Research Council Discovery Project (DP200100965), the Science and Technology Commission of Shanghai Municipality (23520710700), the National Natural Science Foundation of China (22202069), and Griffith University Postdoctoral Fellowship. Cr K-edge and Ni K-edge XAS measurements were performed at the 10-ID-B beamline of the Australian Synchrotron, part of the Australian Nuclear Science and Technology Organization. Cr and Ni L-edge, C, N and O K-edge measurements were performed at the SXR beamline of the Australian Synchrotron. The authors thank Dr Lachlan Casey from The University of Queensland for XPS and FT-EXAFS analysis.

语种：英文

外文关键词：Dual-active-site mechanism; Hydrogen transfer distance; Ni-N3/Cr-N2; Operando XAS and temperature-programmed soft NEXAFS; Zero-gap MEA electrolyzer

摘要：The practical application of electrocatalytic CO2 reduction reaction (CO2RR) holds a great promise but is hindered by low CO2 solubility. Under CO2 mass transfer limitations, the competing hydrogen evolution reaction (HER) is promoted, resulting in a decrease in CO2RR Faradaic efficiency. Before CO2 supply reaches its maximum capacity, in neutral or alkaline conditions, increasing CO2RR selectivity requires additional hydrogen source from solvent H2O dissociation for CO2 protonation. However, it is challenging to concurrently achieve CO2 reduction and H2O dissociation at single active site. Herein, we synthesized a neighboring Ni-Cr atomic pair configuration with distance of similar to 2.7 & Aring;. COMSOL Multiphysics finite-element studies demonstrate that appropriate distance between dual active sites should be on the order of a few angstroms. Operando XAS and soft NEXAFS characterizations indicate that the Ni-N3 promotes CO2 activation and Cr-N2 accelerates H2O dissociation. Theoretical investigations unveil the thermodynamic and kinetic superiorities of dual-active-site mechanism. Ni-N3/Cr-N2 exhibits higher FECO than Ni-N3, whereas Cr-N4 displays a strong preference for HER. The zero-gap MEA attains J of up to -1000 mA cm-2 with a FECO exceeding 85% at a cell voltage of -4.0 V, and maintains stable operation for over 100 h at a J of -200 mA cm-2.