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Selective CO2-to-C2H4 Photoconversion Enabled by Oxygen-Mediated Triatomic Sites in Partially Oxidized Bimetallic Sulfide |
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| Authors: | Yang Wu Prof Qingxia Chen Juncheng Zhu Kai Zheng Mingyu Wu Minghui Fan Prof Wensheng Yan Dr Jun Hu Junfa Zhu Prof Yang Pan Prof Xingchen Jiao Prof Yongfu Sun Yi Xie |
| Institution: | 1. Hefei National Research Center for Physical Sciences at Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, 230026 Hefei, China
These authors contributed equally to this work.;2. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, 214122 Wuxi, China These authors contributed equally to this work.;3. Hefei National Research Center for Physical Sciences at Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, 230026 Hefei, China;4. Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, 214122 Wuxi, China |
| Abstract: | Selective CO2 photoreduction into C2 fuels under mild conditions suffers from low product yield and poor selectivity owing to the kinetic challenge of C?C coupling. Here, triatomic sites are introduced into bimetallic sulfide to promote C?C coupling for selectively forming C2 products. As an example, FeCoS2 atomic layers with different oxidation degrees are first synthesized, demonstrated by X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy spectra. Both experiment and theoretical calculation verify more charges aggregate around the introduced oxygen atom, which enables the original Co?Fe dual sites to turn into Co?O?Fe triatomic sites, thus promoting C?C coupling of double *COOH intermediates. Accordingly, the mildly oxidized FeCoS2 atomic layers exhibit C2H4 formation rate of 20.1 μmol g?1 h?1, with the product selectivity and electron selectivity of 82.9 % and 96.7 %, outperforming most previously reported photocatalysts under similar conditions. |
| Keywords: | C?C Coupling CO2 Photoreduction Partial Oxidation Photocatalysis Triatomic Sites |