Vacancy-defect modulated pathway of photoreduction of CO2 on single atomically thin AgInP2S6 sheets into olefiant gas

• Published in: Nature communications Vol. 12; no. 1; pp. 1 - 8
• Main Authors: Gao, Wa, Li, Shi, He, Huichao, Li, Xiaoning, Cheng, Zhenxiang, Yang, Yong, Wang, Jinlan, Shen, Qing, Wang, Xiaoyong, Xiong, Yujie, Zhou, Yong, Zou, Zhigang
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 06.08.2021; Nature Publishing Group; Nature Portfolio
• Subjects: 639/4077/4057; 639/4077/909/4101/4102; 639/638/77/890; Carbon dioxide; Catalysts; Climate change; Conversion; Coupling (molecular); Crystal defects; Etching; Ethene; Ethylene; Global warming; Humanities and Social Sciences; Hydrocarbon fuels; Hydrogen peroxide; Intermediates; multidisciplinary; Photochemical reactions; Photoreduction; Photosynthesis; Science; Science (multidisciplinary); Selectivity; Sulfur; Thickness; Vacancies
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-021-25068-7

Artificial photosynthesis, light-driving CO 2 conversion into hydrocarbon fuels, is a promising strategy to synchronously overcome global warming and energy-supply issues. The quaternary AgInP 2 S 6 atomic layer with the thickness of ~ 0.70 nm were successfully synthesized through facile ultrasonic exfoliation of the corresponding bulk crystal. The sulfur defect engineering on this atomic layer through a H 2 O 2 etching treatment can excitingly change the CO 2 photoreduction reaction pathway to steer dominant generation of ethene with the yield-based selectivity reaching ~73% and the electron-based selectivity as high as ~89%. Both DFT calculation and in-situ FTIR spectra demonstrate that as the introduction of S vacancies in AgInP 2 S 6 causes the charge accumulation on the Ag atoms near the S vacancies, the exposed Ag sites can thus effectively capture the forming *CO molecules. It makes the catalyst surface enrich with key reaction intermediates to lower the C-C binding coupling barrier, which facilitates the production of ethene. CO 2 conversion driven by light is a promising strategy to synchronously overcome global warming and energy-supply issues. Here the authors show that the sulfur defect engineering on a quaternary AgInP2S6 atomic layer can excitingly change the CO 2 photoreduction reaction pathway to the generation of ethene.