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

doi:10.1021/acsnano.3c10807

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	Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites
	You, Xiao-Meng 1; Xu, Beibei 1; Zhou, Hang 1; Qiao, Hongwei 1; Lv, Xingxi 1; Huang, Zejiang 1; Pang, Jingyi 1; Yang, Lingyun2 ; Liu, Peng Fei 3; Guan, Xiaohong 4; Yang, Hua Gui 3; Wang, Xuelu 1; Yao, Ye-Feng 1
	2024-03-15
发表期刊	ACS NANO (IF:15.8[JCR-2023],16.2[5-Year])
ISSN	1936-0851
EISSN	1936-086X
卷号	18 期号:13 页码:9403-9412
发表状态	已发表
DOI	10.1021/acsnano.3c10807
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 H2 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 dxy and dxz), 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. © 2024 American Chemical Society.
关键词	Atoms Binary alloys Catalyst activity Dimers Nuclear magnetic resonance Photocatalytic activity Platinum Reaction kinetics Reduction Ruthenium Chemical exchange saturation transfer Chemical exchange saturation transfer imaging CO 2 reduction CO2 reduction reaction H 2 evolution Heteronuclear Heteronuclear biatomic atom Reduction reaction Water splitting ]+ catalyst
收录类别	EI
语种	英语
出版者	American Chemical Society
EI入藏号	20241215782998
EI主题词	Carbon dioxide
EI分类号	547.1 Precious Metals ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.2 Inorganic Compounds ; 815.1.1 Organic Polymers ; 931.3 Atomic and Molecular Physics
原始文献类型	Article in Press
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/359933
专题	iHuman研究所 iHuman研究所_公共科研平台_生命科学NMR平台
通讯作者	Wang, Xuelu; Yao, Ye-Feng
作者单位	1.Physics Department, Shanghai Key Laboratory of Magnetic Resonance, School of Physics and Electronic Science, East China Normal University, Shanghai; 200241, China; 2.iHuman Institute, ShanghaiTech University, Shanghai; 201210, China; 3.Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai, Engineering Research Center of Hierarchical Nanomaterials, School of Materials, Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai; 200237, China; 4.Shanghai Engineering Research Center of Biotransformation of Organic Solid Waste, School of Ecological and Environmental Science, East China Normal University, Shanghai; 200241, China
推荐引用方式 GB/T 7714	You, Xiao-Meng,Xu, Beibei,Zhou, Hang,et al. Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites[J]. ACS NANO,2024,18(13):9403-9412.
APA	You, Xiao-Meng.,Xu, Beibei.,Zhou, Hang.,Qiao, Hongwei.,Lv, Xingxi.,...&Yao, Ye-Feng.(2024).Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites.ACS NANO,18(13),9403-9412.
MLA	You, Xiao-Meng,et al."Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites".ACS NANO 18.13(2024):9403-9412.