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

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 ultrasoni...

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Detalles Bibliográficos
Autores principales: Gao, Wa, Li, Shi, He, Huichao, Li, Xiaoning, Cheng, Zhenxiang, Yang, Yong, Wang, Jinlan, Shen, Qing, Wang, Xiaoyong, Xiong, Yujie, Zhou, Yong, Zou, Zhigang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8346554/
https://www.ncbi.nlm.nih.gov/pubmed/34362922
http://dx.doi.org/10.1038/s41467-021-25068-7
Descripción
Sumario: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.