文献类型：期刊文献

英文题名：Engineering Asymmetric Active Sites with Spin Polarization for Selective Photocatalytic CO2-to-CH3COOH Conversion

作者：Wu, Shiqun[1,2];Zhong, Chenggui[1,2];Wang, Lijie[1,2];Yang, Ruijie[1,2];Ye, Ziwei[1,2];He, Chengxuan[1,2];Li, Mingyang[3,4,5];Zhang, Jinlong[1,2]

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]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm, Shanghai 200237, Peoples R China;[3]Natl GoldSun Changzhou Test & Certificat Technol C, Changzhou 213016, Jiangsu, Peoples R China;[4]CNOOC Changzhou Paint & Coatings Ind Res Inst Co L, Changzhou 213016, Jiangsu, Peoples R China;[5]Natl Coating Engn Technol Res Ctr, Changzhou 213016, Jiangsu, Peoples R China

年份：2026

卷号：20

期号：16

起止页码：12357

外文期刊名：ACS NANO

收录：;EI(收录号：20261820602370);WOS:【SCI-EXPANDED(收录号:WOS:001742513500001)】；

基金：This work was supported by the National Natural Science Foundation of China (22572051, 22461142136, 22202070), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (22230780200, 20DZ2250400, 2018SHZDZX03), the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission (24CGA30), and Fundamental Research Funds for the Central Universities (222201717003). We thanks to the Shanghai Synchrotron Radiation Facility of BL14W1 (https://cstr.cn/31124.02.SSRF.BL14W1) for providing beam time. Thanks to the National Synchrotron Radiation Laboratory (NSRL, beamline BL11U) for providing beam time. We thank the staff members of the BL01B beamline (https://cstr.cn/31129.02.NFPS.BL01B) at the National Facility for Protein Science in Shanghai (https://cstr.cn/31129.02.NFPS), for providing technical support and assistance in data collection and analysis.

语种：英文

外文关键词：CO2 photoreduction; Asymmetric active site; Spin polarization; C-C coupling; CH3COOH

摘要：Selective photocatalytic reduction of CO2 to CH3COOH is highly desirable but hindered by poor intermediate stabilization and sluggish C-C coupling. Here we report a coordination-environment engineering strategy to construct asymmetric Co active sites and induce intrinsic spin polarization by nitrogen incorporation into Co3O4. Nitrogen substitution and oxygen vacancy formation generate Co sites with distinct coordination and charge distributions, stabilizing *CO intermediates and lowering the C-C coupling barrier. Concurrently, spin polarization enhances charge carrier separation, further intensified by an external magnetic field. In situ spectroscopy and theoretical calculations confirm the synergistic role of asymmetry and spin effects in facilitating intermediate formation and CH3COOH production. The optimized N-Co3O4-X catalyst achieves a CH3COOH yield of 41.4 mu mol g(-1) h(-1) with 95% electron selectivity under external magnetic field. This work presents a dual-modulation strategy for efficient CO2-to-C-2 conversion.