Tandem Synergistic Effect of Cu‐In Dual Sites Confined on the Edge of Monolayer CuInP2S6 toward Selective Photoreduction of CO2 into Multi‐Carbon Solar Fuels

Author:

Gao Wa12,Shi Li3,Hou Wentao2,Ding Cheng2,Liu Qi4,Long Ran5,Chi Haoqiang2,Zhang Yongcai6,Xu Xiaoyong6,Ma Xueying2,Tang Zheng7,Yang Yong7,Wang Xiaoyong2,Shen Qing8,Xiong Yujie5,Wang Jinlan9,Zou Zhigang4210,Zhou Yong4210ORCID

Affiliation:

1. School of Physical Science and Technology Tiangong University Tianjin 300387 P. R. China

2. School of Physics Jiangsu Key Laboratory of Nanotechnology, Eco-materials and Renewable Energy Research Center (ERERC) National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 P. R. China

3. State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM) Nanjing University of Posts and Telecommunications Nanjing 210023 P. R. China

4. School of Chemical and Environmental Engineering School of Materials and Engineering Anhui Polytechnic University Wuhu 241000 P. R. China

5. School of Chemistry and Materials Science University of Science and Technology of China Hefei 230036 Anhui P. R. China

6. Chemistry Interdisciplinary Research Center School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225009 P. R. China

7. Key Laboratory of Soft Chemistry and Functional Materials (MOE) Nanjing University of Science and Technology Nanjing 210094 P. R. China

8. Graduate School of Informatics and Engineering University of Electrocommunication 1-5-1 Chofugaoka Chofu Tokyo 1828585 Japan

9. School of Physics Southeast University Nanjing 211189 Jiangsu P. R. China

10. School of Science and Engineering The Chinese University of Hongkong (Shenzhen) Shenzhen Guangdong 518172 P. R. China

Abstract

AbstractOne‐unit‐cell, single‐crystal, hexagonal CuInP2S6 atomically thin sheets of≈0.81 nm in thickness was successfully synthesized for photocatalytic reduction of CO2. Exciting ethene (C2H4) as the main product was dominantly generated with the yield‐based selectivity reaching ≈56.4 %, and the electron‐based selectivity as high as ≈74.6 %. The tandem synergistic effect of charge‐enriched Cu−In dual sites confined on the lateral edge of the CuInP2S6 monolayer (ML) is mainly responsible for efficient conversion and high selectivity of the C2H4 product as the basal surface site of the ML, exposing S atoms, can not derive the CO2 photoreduction due to the high energy barrier for the proton‐coupled electron transfer of CO2 into *COOH. The marginal In site of the ML preeminently targets CO2 conversion to *CO under light illumination, and the *CO then migrates to the neighbor Cu sites for the subsequent C−C coupling reaction into C2H4 with thermodynamic and kinetic feasibility. Moreover, ultrathin structure of the ML also allows to shorten the transfer distance of charge carriers from the interior onto the surface, thus inhibiting electron‐hole recombination and enabling more electrons to survive and accumulate on the exposed active sites for CO2 reduction.

Publisher

Wiley

Subject

General Medicine

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