文献类型：期刊文献

英文题名：Symmetry-Differentiated Oxygen-Vacancy Motifs Regulate Au–CeOx Interfaces for Selective Photocatalytic Ethane Production from CO2

作者：Bi, Wei[1]; Meng, Xinhao[1]; Zheng, Yaru[3]; Wu, Shuohan[1]; Zhang, Dongliang[1]; Jiang, Jiechao[2]; Xiao, Shuning[1]; Wang, Mitang[1]; Li, Ying[1]; Wu, Shiqun[4]; Hu, Yanjie[2]; Li, Chunzhong[2]; Zhang, Jinlong[4]

机构：[1] School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai, 200093, China; [2] Shanghai Engineering Research Center of Hierarchical Nanomaterials, Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science & Technology, Shanghai, 200237, China; [3] Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, College of Smart Materials and Future Energy, Fudan University, Shanghai, 200433, China; [4] State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China

年份：2026

卷号：148

期号：28

起止页码：30627

外文期刊名：Journal of the American Chemical Society

收录：EI(收录号：20263021175073);Scopus(收录号：2-s2.0-105045590229)

语种：英文

外文关键词：Cerium - Cerium oxide - Gold - Gold compounds - Hydrocarbons - Hydrogenation - Oxygen - Photocatalytic activity

摘要：Steering CO2 photoreduction toward C2 hydrocarbons remains challenging because of the sluggish multielectron/proton-transfer kinetics and the high energetic demand for C–C coupling. Herein, we report a flame-spray-pyrolysis strategy to construct Au–CeOx nanostructures featuring coexisting symmetric oxygen vacancies (Ce–Ov–Ce) and symmetry-broken oxygen vacancy (Au–Ov–Ce) motifs at the Au–CeOx interface. The symmetric Ce–Ov–Ce sites provide favorable adsorption environments for CO2 activation, whereas the symmetry-broken Au–Ov–Ce sites induce interfacial electron redistribution and promote electron enrichment. The cooperative interaction between these two vacancy configurations shifts the reaction route from *CO desorption toward deep hydrogenation and *CH3-mediated C–C coupling. As a result, the optimized Au–CeOx–SAOv catalyst achieves a C2H6 production rate of 2581 μmol gAu–1 h–1 with a selectivity of 88.14% and an electron utilization rate of 41.22 mmol gAu–1 h–1 in photocatalytic CO2 reduction with H2O. Mechanistic studies suggest that the symmetry-broken Au–Ov–Ce sites stabilize hydrogenated C1 intermediates and lower the energetic requirement for coupling two *CH3 species. This work establishes symmetry-differentiated oxygen-vacancy engineering as an effective strategy for directing multielectron CO2 photoreduction toward C2 hydrocarbons. ? 2026 American Chemical Society