文献类型：期刊文献

英文题名：Synergistic regulation of oxygen vacancies and Zr-O-Cu motifs for selective C-C coupling

作者：Zhang, Yu[1];Geng, Shuchen[1];Chen, Cheng[1];Zhang, Mingliang[1];Wei, Hehe[2];Wang, Haifeng[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Tsinghua Univ, Sch Mat Sci & Engn, State Key Lab New Ceram Mat, Beijing 100084, Peoples R China

年份：2026

卷号：60

外文期刊名：MATERIALS TODAY ENERGY

收录：;EI(收录号：20262320855480);WOS:【SCI-EXPANDED(收录号:WOS:001792157000001)】；

基金：This study was supported by the National Key R & D Program of China (2021YFA1500700) and the National Nature Science Foundation of China (22102057, 22203030, 22525202, 12104235, 22473043, 52302058) . The authors thank the Research Center of Analysis and Test of East China University of Science and Technology and the Feringa Nobel Prize Scientist Joint Research Center for the characterizations.

语种：英文

外文关键词：CO2RR; Cu2O; Electrocatalysis; Multicarbon (C2+) products

摘要：Achieving selective electrochemical CO2 reduction to multicarbon (C2+) products is severely impeded by sluggish C-C coupling and uncontrolled proton-coupled electron transfer pathways. Herein, we report a robust defect-engineering strategy via Zr incorporation into Cu2O (Zrx-Cu2O) to construct a bifunctional catalytic platform featuring tailored oxygen vacancies and stable Zr-O-Cu interfacial motifs. Zr doping induces lattice contraction and localized charge redistribution, which simultaneously populates interfacial oxygen vacancies and immobilizes active Cu+ species against cathodic over-reduction. Spectroscopic and theoretical analyses reveal that this synergy drives a pivotal pathway shift: the oxygen vacancies drastically accelerate H2O dissociation to supply sufficient protons for *COH generation, while the adjusted electronic structure promotes energetically favorable asymmetric *CO-*COH coupling over conventional symmetric CO dimerization. Consequently, the optimized Zr0.10-Cu2O catalyst delivers an outstanding C2+ Faradaic efficiency of 75.4 +/- 1.2% at a high current density of 300 mA cm-2 with exceptional operational stability exceeding 360 min in situ ATR-SEIRAS captures the crucial *OCCOH intermediate, validating that defect-coordination synergy offers a powerful paradigm for governing reaction pathways toward high-rate multicarbon synthesis.