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In-plane heterostructured Ag2S-In2S3 atomic layers enabling boosted CO2 photoreduction into CH4

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Abstract

Sluggish separation and migration kinetics of the photogenerated carriers account for the low-efficiency of CO2 photoreduction into CH4. Design and construction two-dimensional (2D) in-plane heterostructures demonstrate to be an appealing approach to address above obstacles. Herein, we fabricate 2D in-plane heterostructured Ag2S-In2S3 atomic layers via an ion-exchange strategy. Photoluminescence spectra, time-resolved photoluminescence spectra, and photoelectrochemical measurements firmly affirm the optimized carrier dynamics of the In2S3 atomic layers after the introduction of in-plane heterostructure. In-situ Fourier transform infrared spectroscopy spectra and density functional theory (DFT) calculations disclose the in-plane heterostructure contributes to CO2 activation and modulates the adsorption strength of CO* intermediates to facilitate the formation of CHO* intermediates, which are further protonated to CH4. In consequence, the in-plane heterostructure achieves the CH4 evolution rate of 20 µmol·g−1·h−1, about 16.7 times higher than that of the In2S3 atomic layers. In short, this work proves construction of in-plane heterostructures as a promising method for obtaining high-efficiency CO2-to-CH4 photoconversion properties.

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Acknowledgements

This work was financially supported by the National Key R&D Program of China (Nos. 2019YFA0210004, 2017YFA0207301, and 2017YFA0303500), the National Natural Science Foundation of China (Nos. 21975242, U2032212, 21890754, and 21805267), the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000), Youth Innovation Promotion Association of CAS (No. CX2340007003), Major Program of Development Foundation of Hefei Center for Physical Science and Technology (No. 2020HSC-CIP003), Key Research Program of Frontier Sciences of CAS (No. QYZDY-SSW-SLH011), the Fok Ying-Tong Education Foundation (No. 161012), the University Synergy Innovation Program of Anhui Province (GXXT-2020-001), and Users with Excellence Program of Hefei Science Center CAS (2020HSC-UE001). Supercomputing USTC and National Supercomputing Center in Shenzhen are acknowledged for computational support.

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  1. Weiwei Shao, Shumin Wang, and Juncheng Zhu contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory for Physical Sciences at Microscale, CAS Centre for Excellence in Nanoscience, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China

    Weiwei Shao, Shumin Wang, Juncheng Zhu, Xiaodong Li, Xingchen Jiao, Yang Pan, Yongfu Sun & Yi Xie

  2. Institute of Energy, Hefei Comprehensive National Science Center, Hefei, 230031, China

    Yongfu Sun & Yi Xie

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  1. Weiwei Shao
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  4. Xiaodong Li
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Correspondence to Yongfu Sun.

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Shao, W., Wang, S., Zhu, J. et al. In-plane heterostructured Ag2S-In2S3 atomic layers enabling boosted CO2 photoreduction into CH4. Nano Res. 14, 4520–4527 (2021). https://doi.org/10.1007/s12274-021-3365-4

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