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Research Article

MoC nanocrystals confined in N-doped carbon nanosheets toward highly selective electrocatalytic nitric oxide reduction to ammonia

Ge Meng1,§( ), Mengmeng Jin2,§, Tianran Wei3,§, Qian Liu4, Shusheng Zhang5, Xianyun Peng6( ), Jun Luo2, Xijun Liu3( )
Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, 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
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 Advanced Study, Chengdu University, Chengdu 610106, China
College of Chemistry, Zhengzhou University, Zhengzhou 450000, China
Institute of Zhejiang University–Quzhou, Quzhou 324000, China

§ Ge Meng, Mengmeng Jin, and Tianran Wei contributed equally to this work.

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Graphical Abstract

Electrochemical nitric oxide reduction reaction (NORR) to produce ammonia (NH3) under ambient conditions is a promising alternative to the energy and carbon-intensive Haber–Bosch approach, but its performance is still improved. Herein, molybdenum carbides (MoC) nanocrystals confined by nitrogen-doped carbon nanosheets are first designed as an efficient and durable electrocatalyst for catalyzing the reduction of NO to NH3 with maximal Faradaic efficiency of 89% ± 2% and a yield rate of 1,350 ± 15 μg·h−1·cm−2 at the applied potential of −0.8 V vs. reversible hydrogen electrode (RHE) as well as high stable activity with negligible current density and NH3 yield rate decays over a 30 h continue the test. Moreover, as a proof-of-concept of Zn–NO battery, it achieves a peak power density of 1.8 mW·cm−2 and a large NH3 yield rate of 782 ± 10 μg·h−1·cm−2, which are comparable to the best-reported results. Theoretical calculations reveal that the MoC(111) has a strong electronic interaction with NO molecules and thus lowering the energy barrier of the potential-determining step and suppressing hydrogen evolution kinetics. This work suggests that Mo-based materials are a powerful platform providing great opportunities to explore highly selective and active catalysts for NH3 production.

Abstract

Electrochemical nitric oxide reduction reaction (NORR) to produce ammonia (NH3) under ambient conditions is a promising alternative to the energy and carbon-intensive Haber–Bosch approach, but its performance is still improved. Herein, molybdenum carbides (MoC) nanocrystals confined by nitrogen-doped carbon nanosheets are first designed as an efficient and durable electrocatalyst for catalyzing the reduction of NO to NH3 with maximal Faradaic efficiency of 89% ± 2% and a yield rate of 1,350 ± 15 μg·h−1·cm−2 at the applied potential of −0.8 V vs. reversible hydrogen electrode (RHE) as well as high stable activity with negligible current density and NH3 yield rate decays over a 30 h continue the test. Moreover, as a proof-of-concept of Zn–NO battery, it achieves a peak power density of 1.8 mW·cm−2 and a large NH3 yield rate of 782 ± 10 μg·h−1·cm−2, which are comparable to the best-reported results. Theoretical calculations reveal that the MoC(111) has a strong electronic interaction with NO molecules and thus lowering the energy barrier of the potential-determining step and suppressing hydrogen evolution kinetics. This work suggests that Mo-based materials are a powerful platform providing great opportunities to explore highly selective and active catalysts for NH3 production.

Keywords

ammonia electrosynthesisgreen routemolybdenum carbides (MoC) nanocrystalsnitric oxide reduction reactionhigh selectivity

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Nano Research
Volume 15 Issue 10,
October 2022
Pages 8890-8896
DOI: 10.1007/s12274-022-4747-y
Cite this article:
Meng G, Jin M, Wei T, et al. MoC nanocrystals confined in N-doped carbon nanosheets toward highly selective electrocatalytic nitric oxide reduction to ammonia. Nano Research, 2022, 15(10): 8890-8896. https://doi.org/10.1007/s12274-022-4747-y
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Received: 20 May 2022
Revised: 24 June 2022
Accepted: 07 July 2022
Published: 18 August 2022
© Tsinghua University Press 2022
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