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Nano Research 2023, 16(4): 5743-5749 https://doi.org/10.1007/s12274-022-5246-x
Research Article | Issue | Published: 23 November 2022

Coupling Fe and Mo single atoms on hierarchical N-doped carbon nanotubes enhances electrochemical nitrogen reduction reaction performance

Show Author's Information Wenjie Cui1,2,  Baokang Geng1,2,  Xiang Chu1,2,  Jianing He1,2,  Lingxi Jia1,2,  Xiaoxiao Han1,2,  Xiao Wang1,2( ),  Shuyan Song1,2( ),  Hongjie Zhang1,2,3( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Keywords:
hard template, synergetic effect, single atom, nitrogen reduction reaction (NRR), dual-site
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Cui W, Geng B, Chu X, et al. Coupling Fe and Mo single atoms on hierarchical N-doped carbon nanotubes enhances electrochemical nitrogen reduction reaction performance. Nano Research, 2023, 16(4): 5743-5749. https://doi.org/10.1007/s12274-022-5246-x
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Abstract Full text Electronic supplementary material About this article

Electrochemical nitrogen reduction reaction (NRR) paves a new way to cost-efficient production of ammonia, but is still challenging in the sluggish kinetics caused by hydrogen evolution reaction competition and chemical inertness of N≡N bond. Herein, we report a “dual-site” strategy for boosting NRR performance. A high-performance catalyst is successfully constructed by anchoring isolated Fe and Mo atoms on hierarchical N doped carbon nanotubes through a facile self-sacrificing template route, which exhibits a remarkably improved NH3 yield rate of 26.8 μg·h−1·mg cat.−1 with 11.8% Faradaic efficiency, which is 2.5 and 1.6 times larger than those of Fe/NC and Mo/NC. The enhancement can be attributed to the unique hierarchical structure that profits from the contact of electrode and electrolyte, thus improving the mass and electron transport. More importantly, the in situ Fourier transform infrared spectroscopy (in situ FTIR) result firmly demonstrates the crucial role of the coupling of Fe and Mo atoms, which can efficiently boost the generation and transmission of *N2Hy intermediates, leading to an accelerated reaction rate.


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Electronic supplementary material
About this article

Coupling Fe and Mo single atoms on hierarchical N-doped carbon nanotubes enhances electrochemical nitrogen reduction reaction performance

Show Author's information Wenjie Cui1,2, Baokang Geng1,2, Xiang Chu1,2, Jianing He1,2, Lingxi Jia1,2, Xiaoxiao Han1,2, Xiao Wang1,2( ), Shuyan Song1,2( ), Hongjie Zhang1,2,3( )
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

Abstract

Electrochemical nitrogen reduction reaction (NRR) paves a new way to cost-efficient production of ammonia, but is still challenging in the sluggish kinetics caused by hydrogen evolution reaction competition and chemical inertness of N≡N bond. Herein, we report a “dual-site” strategy for boosting NRR performance. A high-performance catalyst is successfully constructed by anchoring isolated Fe and Mo atoms on hierarchical N doped carbon nanotubes through a facile self-sacrificing template route, which exhibits a remarkably improved NH3 yield rate of 26.8 μg·h−1·mg cat.−1 with 11.8% Faradaic efficiency, which is 2.5 and 1.6 times larger than those of Fe/NC and Mo/NC. The enhancement can be attributed to the unique hierarchical structure that profits from the contact of electrode and electrolyte, thus improving the mass and electron transport. More importantly, the in situ Fourier transform infrared spectroscopy (in situ FTIR) result firmly demonstrates the crucial role of the coupling of Fe and Mo atoms, which can efficiently boost the generation and transmission of *N2Hy intermediates, leading to an accelerated reaction rate.

Keywords: hard template, synergetic effect, single atom, nitrogen reduction reaction (NRR), dual-site

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Publication history
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Acknowledgements

Publication history

Received: 14 September 2022
Revised: 22 October 2022
Accepted: 25 October 2022
Published: 23 November 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the financial aid from National Science and Technology Major Project of China (No. 2021YFB3500700), National Natural Science Foundation of China (Nos. 22020102003, 22025506, and 22271274), Key Research Program of the Chinese Academy of Sciences (No. ZDRW-CN-2021-3-3), K. C. Wong Education Foundation (No. GJTD-2018-09), and Innovation and Entrepreneurship Program of Jilin Province (No. E2390202).

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