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Electrocatalytic NO reduction reaction to generate NH3 under ambient conditions offers an attractive alternative to the energy-extensive Haber–Bosch route; however, the challenge still lies in the development of cost-effective and high-performance electrocatalysts. Herein, nanoporous VN film is first designed as a highly selective and stable electrocatalyst for catalyzing reduction of NO to NH3 with a maximal Faradaic efficiency of 85% and a peak yield rate of 1.05 × 10–7 mol·cm–2·s–1 (corresponding to 5,140.8 μg·h–1·mgcat.–1) at –0.6 V vs. reversible hydrogen electrode in acid medium. Meanwhile, this catalyst maintains an excellent activity with negligible current density and NH3 yield rate decays over 40 h. Moreover, as a proof-of-concept of Zn–NO battery, it delivers a high power density of 2.0 mW·cm–2 and a large NH3 yield rate of 0.22 × 10–7 mol·cm–2·s–1 (corresponding to 1,077.1 μg·h–1·mgcat.–1), both of which are comparable to the best-reported results. Theoretical analyses confirm that the VN surface favors the activation and hydrogenation of NO by suppressing the hydrogen evolution. This work highlights that the electrochemical NO reduction is an eco-friendly and energy-efficient strategy to produce NH3.


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High-efficiency electrocatalytic NO reduction to NH3 by nanoporous VN

Show Author's information Defeng Qi1,2,§Fang Lv2,§Tianran Wei1,§Mengmeng Jin2Ge Meng3Shusheng Zhang4Qian Liu5Wenxian Liu6Dui Ma1Mohamed S. Hamdy7Jun Luo2Xijun Liu1( )
MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials, and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resource, Environments and Materials, Guangxi University, Nanning 530004, China
Institute for New Energy Materials and Low-Carbon Technologies, Tianjin Key Lab for Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China
College of Chemistry, Zhengzhou University, Zhengzhou 450000, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China
Catalysis Research Group (CRG), Department of Chemistry, College of Science, King Khalid University, P.O. Box 9004, 61413 Abha, Saudi Arabia

§Defeng Qi, Fang Lv, and Tianran Wei contributed equally to this work.

Abstract

Electrocatalytic NO reduction reaction to generate NH3 under ambient conditions offers an attractive alternative to the energy-extensive Haber–Bosch route; however, the challenge still lies in the development of cost-effective and high-performance electrocatalysts. Herein, nanoporous VN film is first designed as a highly selective and stable electrocatalyst for catalyzing reduction of NO to NH3 with a maximal Faradaic efficiency of 85% and a peak yield rate of 1.05 × 10–7 mol·cm–2·s–1 (corresponding to 5,140.8 μg·h–1·mgcat.–1) at –0.6 V vs. reversible hydrogen electrode in acid medium. Meanwhile, this catalyst maintains an excellent activity with negligible current density and NH3 yield rate decays over 40 h. Moreover, as a proof-of-concept of Zn–NO battery, it delivers a high power density of 2.0 mW·cm–2 and a large NH3 yield rate of 0.22 × 10–7 mol·cm–2·s–1 (corresponding to 1,077.1 μg·h–1·mgcat.–1), both of which are comparable to the best-reported results. Theoretical analyses confirm that the VN surface favors the activation and hydrogenation of NO by suppressing the hydrogen evolution. This work highlights that the electrochemical NO reduction is an eco-friendly and energy-efficient strategy to produce NH3.

Keywords:

NH3 electrosynthesis, green route, nanoporous VN, NO reduction reaction, high-performance
Received: 28 May 2022 Revised: 29 June 2022 Accepted: 30 June 2022 Published: 07 July 2022 Issue date: September 2022
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Publication history

Received: 28 May 2022
Revised: 29 June 2022
Accepted: 30 June 2022
Published: 07 July 2022
Issue date: September 2022

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© The Author(s) 2022. Published by Tsinghua University Press.

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22075211, 22109118, 21601136, 51971157, 51621003, and 21905246), and Tianjin Science Fund for Distinguished Young Scholars (No. 19JCJQJC61800). The authors would also like to express their gratitude to Deanship of Scientific Research at King Khalid University, Abha, Saudi Arabia for funding this work through the Research Group Program under No. RGP.2/79/43.

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