Issue 14, 2024

Constructing asymmetric dual active sites through symbiotic effect for achieving efficient and selective photoreduction of CO2 to C2H4

Abstract

One of the biggest obstacles to the light-driven conversion of greenhouse gas CO2 into high value-added multi-carbon compounds is manipulating the C–C coupling reaction. Herein, we propose using a symbiotic effect to construct asymmetric dual active sites, namely doping CuInS2 (CIS) with single atomic Ag, accompanied by the formation of sulfur vacancies (Sv). Thus, Sv and the neighbouring In metal atom double sites are constructed, and CO2 photoreduction products undergo a transformation from C1 products to C2H4. Meanwhile, the doped Ag plays a role in capturing and transferring photogenerated electrons, improving the reduction rate. The generation rate of C2H4 is 53.8 μmol g−1 h−1 with a selectivity of 98.8%. Based on the number of transferred electrons, the catalytic activity of 2%Ag/CuInS2 (2%Ag/CIS) is 90 times that of CIS. Experimental and theoretical calculations verify that the key intermediates *CO and *CHO adsorbed on Sv and In sites, respectively, are propitious to promote the occurrence of the C–C coupling reaction owing to the reasonable distance, asymmetric electron distribution and distinct adsorption capacity. Accordingly, the findings provide a new strategy for designing asymmetric catalytic active sites for the selective photosynthesis of multi-carbon products from CO2.

Graphical abstract: Constructing asymmetric dual active sites through symbiotic effect for achieving efficient and selective photoreduction of CO2 to C2H4

Supplementary files

Article information

Article type
Paper
Submitted
27 Mar 2024
Accepted
31 May 2024
First published
01 Jun 2024

Energy Environ. Sci., 2024,17, 5060-5069

Constructing asymmetric dual active sites through symbiotic effect for achieving efficient and selective photoreduction of CO2 to C2H4

Y. Xu, P. Wang, M. Zhang, W. Dai, Y. Xu, J. Zou and X. Luo, Energy Environ. Sci., 2024, 17, 5060 DOI: 10.1039/D4EE01376J

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