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Theory assisted design of N-doped tin oxides for enhanced electrochemical CO2 activation and reduction

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Abstract

Clearly understanding the structure-function relationship and rational design of efficient CO2 electrocatalysts are still the challenges. This article describes the molecular origin of high selectivity of formic acid on N-doped SnO2 nanoparticles, which obtained via thermal treatment of g-C3N4 and SnCl2·2H2O precursor. Combined with density functional theory (DFT) calculations, we discover that N-doping effectively introduces oxygen vacancies and increases the charge density of Sn sites, which plays a positive role in CO2 activation. In addition, N-doping further regulates the adsorption energy of *OCHO, *COOH, *H and promotes HCOOH generation. Benefited from above modulation, the obtained N-doped SnO2 catalysts with oxygen vacancies (Ov-N-SnO2) exhibit faradaic efficiency of 93% for C1 formation, 88% for HCOOH production and well-suppression of H2 evolution over a wide range of potentials.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2016YFB0600901), the National Natural Science Foundation of China (21525626, 21606169, 21722608), and the Program of Introducing Talents of Discipline to Universities (B06006).

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Authors and Affiliations

  1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University; Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China

    Congling Hu, Lei Zhang, Lulu Li, Wenjin Zhu, Wanyu Deng, Hao Dong, Zhi-Jian Zhao & Jinlong Gong

  2. Department of Mechanical and Materials Engineering, Western University, London, ON, N6A 5B9, Canada

    Lei Zhang

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  1. Congling Hu
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  2. Lei Zhang
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  3. Lulu Li
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  5. Wanyu Deng
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  6. Hao Dong
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  7. Zhi-Jian Zhao
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  8. Jinlong Gong
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Correspondence to Jinlong Gong.

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Hu, C., Zhang, L., Li, L. et al. Theory assisted design of N-doped tin oxides for enhanced electrochemical CO2 activation and reduction. Sci. China Chem. 62, 1030–1036 (2019). https://doi.org/10.1007/s11426-019-9474-0

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  • DOI: https://doi.org/10.1007/s11426-019-9474-0

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