文献类型：期刊文献

英文题名：Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites

作者：You, Xiao-Meng[1,2];Xu, Beibei[1,2];Zhou, Hang[1,2];Qiao, Hongwei[1,2];Lv, Xingxi[1,2];Huang, Zejiang[1,2];Pang, Jingyi[1,2];Yang, Lingyun[3];Liu, Peng Fei[4];Guan, Xiaohong[5];Yang, Hua Gui[4];Wang, Xuelu[1,2];Yao, Ye-Feng[1,2]

机构：[1]East China Normal Univ, Sch Phys & Elect Sci, Phys Dept, Shanghai 200241, Peoples R China;[2]East China Normal Univ, Sch Phys & Elect Sci, Shanghai Key Lab Magnet Resonance, Shanghai 200241, Peoples R China;[3]ShanghaiTech Univ, iHuman Inst, Shanghai 201210, Peoples R China;[4]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[5]East China Normal Univ, Shanghai Engn Res Ctr Biotransformat Organ Solid W, Sch Ecol & Environm Sci, Shanghai 200241, Peoples R China

年份：2024

卷号：18

期号：13

起止页码：9403

外文期刊名：ACS NANO

收录：;EI(收录号：20241215782998);WOS:【SCI-EXPANDED(收录号:WOS:001186348000001)】；

基金：This work was supported by the National Natural Science Foundation of China (Grants 22072045 and 21574043), the Ministry of Science and Technology of the People's Republic of China (Grant 2018YFC1602800), XingFu-Zhi-Hua Foundation of ECNU, the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the Science and Technology Commission of Shanghai Municipality (21DZ1207101) and Microscale Magnetic Resonance Platform of ECNU.

语种：英文

外文关键词：heteronuclear biatomic atom; chemical exchangesaturationtransfer (CEST) imaging; CO2 reduction reaction; water splitting; photocatalysis

摘要：Diatomic-site catalysts (DASCs) inherit the excellent performance of single-atom catalysts (SACs) by utilizing two adjacent atomic metal species to achieve functional complementarity and synergistic effects that improve the carbon dioxide reduction reaction (CO2RR) and H-2 evolution reaction (HER) kinetics. Herein, we report a method to further improve the catalytic efficiency of Pt by using Pt and Ru single atoms randomly anchored on a g-C3N4 surface, yielding partial Pt-Ru dimers. The synthesized catalyst exhibits extraordinary photocatalytic activity and stability in both the CO2RR and HER processes. In-depth experimentation, the pH-dependent chemical exchange saturation transfer (CEST) imaging nuclear magnetic resonance (NMR) method, and theoretical analyses reveal that the excellent performance is attributed to orbital coupling between the Pt atoms and the neighboring Ru atoms (mainly d( xy )and d( xz )), which decreases the orbital energy levels and weakens the bond strength with intermediates, resulting in improved CO2RR and HER performance. This study successfully applies the pH-dependent CEST imaging NMR method to catalytic reactions, and CO2 adsorption is directly observed using CEST 2D imaging maps. This work presents significant potential for a variety of catalytic reaction applications by systematically designing bimetallic dimers with higher activity and stability.