文献类型：期刊文献

英文题名：Spatially Separated C-C Coupling and Protonation on Cl-Bridged Ti-Ag Dual-Site Catalysts for Efficient Photocatalytic CO2 Reduction to C2H4

作者：Du, Haoran[1,2,3];Fu, Yangjie[4];Shi, Rou[3];Cao, Zhiyang[3];Zhang, Shao[5];Liu, Kaihong[3];Wang, Jiaqi[1,2,3];Jiang, Bo[3];Li, Hexing[1,2,3,6]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]Shanghai Normal Univ, Joint Int Res Lab Resource Chem, Key Lab Resource Chem,Shanghai Frontiers Sci Ctr B, Coll Chem & Mat Sci,Educ Minist,Shanghai Key Lab R, Shanghai 200234, Peoples R China;[4]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[5]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China;[6]Shanghai Res Inst Chem Ind Co Ltd, State Key Lab Polyolefins & Catalysis, Shanghai Key Lab Catalysis Technol Polyolefins, Shanghai 200062, Peoples R China

年份：2026

卷号：65

期号：3

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20254819578770);WOS:【SCI-EXPANDED(收录号:WOS:001619235300001)】；

基金：This work was supported by the National Key Research and Development Program of China (2020YFA0211004), the National Natural Science Foundation of China (22236005, 22576138), the Foundation from Shanghai Local Government (25ZR1401276, 22010503400, and 23520711100), the Shanghai Engineering Research Center of Green Energy Chemical Engineering and State Key Laboratory of Chemical Engineering and Low-Carbon Technology (SKL-ChE-23C04) and State Key Laboratory of Polyolefins and Catalysis and Shanghai Key Laboratory of Catalysis Technology for Polyolefins (SKL-LCTP-202403).

语种：英文

外文关键词：C-C Coupling; Cl-bridged dual-site; Single-atom catalyst; Photocatalytic CO2 reduction

摘要：Solar-driven selective reduction of CO2 to C2H4 conversion is bottlenecked by the concurrent demands for intermediate protonation and C-C coupling. Herein, we constructed a chlorine (Cl)-bridged Ti-Ag dual-site catalysts to overcome above issues. The introduction of Cl on Ti-Ag dual sites spatially separates C-C coupling and intermediate protonation, making *CO dimerization thermodynamically more favorable than *CO hydrogenation. In situ characterization and DFT calculations reveal that the Cl enables the Ti sites within the Ti & horbar;Cl & horbar;Ag configuration act as active center for CO2 activation and C-C coupling, thereby increasing the *CO intermediate concentration and lowering the C-C coupling energy barrier. Concurrently, Ag sites preferentially catalyze H2O dissociation, providing active hydrogen for the subsequent protonation of *OCCO intermediates, thus increasing the overall C2H4 formation rate. The optimized Ti & horbar;Cl & horbar;Ag catalysts achieve high C2H4 production rate of 244 mu molg-1h-1 with 64.3% selectivity, outperforming O-bridged Ti-Ag catalysts which mainly favor *CO deep hydrogenation. This work establishes spatially separated Ti-Ag dual sites that orchestrates site-specific C-C coupling and active hydrogen feeding, providing a rational design concept of photocatalysts for selective reduction of CO2 to C2H4.