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Fe-doped SnO2 nanosheet for ambient electrocatalytic nitrogen reduction reaction

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Abstract

Ammonia plays a vital role in the development of modern agriculture and industry. Compared to the conventional Haber—Bosch ammonia synthesis in industry, electrocatalytic nitrogen reduction reaction (NRR) is considered as a promising and environmental friendly strategy to synthesize ammonia. Here, inspired by biological nitrogenase, we designed iron doped tin oxide (Fe-doped SnO2) for nitrogen reduction. In this work, iron can optimize the interface electron transfer and improve the poor conductivity of the pure SnO2, meanwhile, the synergistic effect between iron and Sn ions improves the catalyst activity. In the electrocatalytic NRR test, Fe-doped SnO2 exhibits a NH3 yield of 28.45 μg·h−1mg −1cat , which is 2.1 times that of pure SnO2, and Faradaic efficiency of 6.54% at −0.8 V vs. RHE in 0.1 M Na2SO4. It also shows good stability during a 12-h long-term stability test. Density functional theory calculations show that doped Fe atoms in SnO2 enhance catalysis performance of some Sn sites by strengthening N—Sn interaction and lowering the energy barrier of the rate-limiting step of NRR. The transient photovoltage test reveals that electrons in the low-frequency region are the key to determining the electron transfer ability of Fe-doped SnO2.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51802126 and 52072152), the Jiangsu University Jinshan Professor Fund and the Jiangsu Specially-Appointed Professor Fund, Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials, and the Science and Technology Planning Social Development Project of Zhenjiang City (No. SH2019010).

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  1. Yaxi Li and Yixian Liu contributed equally to this work.

Authors and Affiliations

  1. Institute for Energy Research, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China

    Yaxi Li, Yixian Liu, Yunliang Liu, Yuanyuan Cheng, Peiji Deng, Jiujun Deng & Haitao Li

  2. Institute of Medicine & Chemical Engineering, Zhenjiang College, Zhenjiang, 212000, China

    Xiang Liu

  3. Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou, 510006, China

    Peng Zhang

  4. School of Physics, The University of Sydney, Sydney, New South Wales, 2006, Australia

    Peng Zhang

  5. Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices, Soochow University, Suzhou, 215123, China

    Zhenhui Kang

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  1. Yaxi Li
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Li, Y., Liu, Y., Liu, X. et al. Fe-doped SnO2 nanosheet for ambient electrocatalytic nitrogen reduction reaction. Nano Res. 15, 6026–6035 (2022). https://doi.org/10.1007/s12274-022-4298-2

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