文献类型：期刊文献

英文题名：Orbital Matching Mechanism-Guided Synthesis of Cu-Based Single Atom Alloys for Acidic CO2 Electroreduction

作者：Xu, Yi Ning[1];Li, Jia-hui[2,3];Wu, Jia Chen[1];Li, Wenbo[4,5];Yang, Yuwei[6];Wu, Haoran[7];Fu, Huai Qin[8];Zhu, Minghui[7];Wang, Xue Lu[9,10];Dai, Sheng[4,5];Lian, Cheng[2];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Shenzhen Univ Adv Technol, Fac Synthet Biol, Shenzhen 518107, Peoples R China;[4]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[6]Univ New South Wales, Sch Chem Engn, Sydney, NSW 2052, Australia;[7]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[8]Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[9]East China Normal Univ, Sch Phys & Elect Sci, Phys Dept, Shanghai 200062, Peoples R China;[10]East China Normal Univ, Sch Phys & Elect Sci, Shanghai Key Lab Magnet Resonance, Shanghai 200062, Peoples R China

年份：2025

卷号：37

期号：18

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20251318121978);WOS:【SCI-EXPANDED(收录号:WOS:001447964900001)】；

基金：Y.N.X. and J.L. contributed equally to this work. This work was financially supported by the National Key Research and Development Program of China (No: 2023YFA1507102), the National Natural Science Foundation of China (22239001 and 22379043), the Shanghai Pilot Program for Basic Research (22TQ1400100-12), the Science and Technology Commission of Shanghai Municipality (23520710700) and the Fundamental Research Funds for the Central Universities. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, the crew of the BL 14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF), and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses. The authors also thank the Jiaxing Puxiang Technology Co. Ltd. for the helpful test and discussion of in situ ATR-SEIRAS results.

语种：英文

外文关键词：acid CO2 electroreduction; orbital matching mechanism; single atom alloy; synthesis

摘要：Recent advancements in alloy catalysis have yield novel materials with tailored functionalities. Among these, Cu-based single-atom alloy (SAA) catalysts have attracted significant attention in catalytic applications for their unique electronic structure and geometric ensemble effects. However, selecting alloying atoms with robust dispersion stability on the Cu substrate is challenging, and has mostly been practiced empirically. The fundamental bottleneck is that the microscopic mechanism that governs the dispersion stability is unclear, and a comprehensive approach for designing Cu-based SAA systems with simultaneous dispersion stability and high catalytic activity is still missing. Here, combining theory and experiment, a simple yet intuitive d-p orbital matching mechanism is discovered for rapid assessment of the atomic dispersion stability of Cu-based SAAs, exhibiting its universality and extensibility for screening effective SAAs across binary, ternary and multivariant systems. The catalytic selectivity of the newly designed SAAs is demonstrated in a prototype reaction-acidic CO2 electroreduction, where all SAAs achieve single-carbon product selectivity exceeding 70%, with Sb1Cu reaching a peak CO faradaic efficiency of 99.73 +/- 2.5% at 200 mA cm(-2). This work establishes the fundamental design principles for Cu-based SAAs with excellent dispersion stability and selectivity, and will boost the development of ultrahigh-performance SAAs for advanced applications such as electrocatalysis.