Vacancy-defect modulated pathway of photoreduction of CO 2 on single atomically thin AgInP 2 S 6 sheets into olefiant gas

• Published in: Nature communications 2021-08, Vol.12 (1), p.4747
• 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: Article
• Language: English
• ISSN: 2041-1723
• DOI: 10.1038/s41467-021-25068-7

Artificial photosynthesis, light-driving CO conversion into hydrocarbon fuels, is a promising strategy to synchronously overcome global warming and energy-supply issues. The quaternary AgInP S 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 O etching treatment can excitingly change the CO 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 S 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.