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

Wa Gao, Shi Li, Huichao He, Xiaoning Li, Zhenxiang Cheng, Yong Yang, Jinlan Wang (), Qing Shen, Xiaoyong Wang, Yujie Xiong (), Yong Zhou () and Zhigang Zou
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Wa Gao: Nanjing University
Shi Li: Southeast University
Huichao He: Southwest University of Science and Technology
Xiaoning Li: University of Wollongong, Squires Way
Zhenxiang Cheng: University of Wollongong, Squires Way
Yong Yang: Nanjing University of Science and Technology
Jinlan Wang: Southeast University
Qing Shen: University of Electrocommunication, Grad Sch Informatics and Engineering
Xiaoyong Wang: Nanjing University
Yujie Xiong: University of Science and Technology of China
Yong Zhou: Nanjing University
Zhigang Zou: Nanjing University

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Artificial photosynthesis, light-driving CO2 conversion into hydrocarbon fuels, is a promising strategy to synchronously overcome global warming and energy-supply issues. The quaternary AgInP2S6 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 H2O2 etching treatment can excitingly change the CO2 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 AgInP2S6 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.

Date: 2021
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DOI: 10.1038/s41467-021-25068-7

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