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Industrial-scale ammonia (NH3) production mainly relies on the energy-intensive and environmentally unfriendly Haber-Bosch process. Such issue can be avoided by electrocatalytic N2 reduction which however suffers from limited current efficiency and NH3 yield. Herein, we demonstrate ambient NH3 production via electrochemical nitrite (NO2) reduction catalyzed by a CoP nanoarray on titanium mesh (CoP NA/TM). When tested in 0.1 M PBS (pH = 7) containing 500 ppm NO2, such CoP NA/TM is capable of affording a large NH3 yield of 2, 260.7 ± 51.5 μg·h–1·cm–2 and a high Faradaic efficiency of 90.0 ± 2.3% at –0.2 V vs. a reversible hydrogen electrode. Density functional theory calculations reveal that the potential-determining step for NO2 reduction over CoP (112) is *NO2 → *NO2H.


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Ambient ammonia production via electrocatalytic nitrite reduction catalyzed by a CoP nanoarray

Show Author's information Guilai Wen1Jie Liang2Qian Liu3Tingshuai Li2Xuguang An3Fang Zhang4Abdulmohsen Ali Alshehri5Khalid Ahmed Alzahrani5Yonglan Luo1( )Qingquan Kong3( )Xuping Sun2( )
Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province School of Chemistry and Chemical Engineering China West Normal University Nanchong 637002 China
Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 610054 China
Institute for Advanced Study Chengdu University Chengdu 610106 China
National Engineering Research Center for Nanotechnology No. 28 East Jiang Chuan Road Shanghai 200241 China
Chemistry Department Faculty of Science King Abdulaziz University P.O. Box 80203 Jeddah, 21589, Saudi Arabia

Abstract

Industrial-scale ammonia (NH3) production mainly relies on the energy-intensive and environmentally unfriendly Haber-Bosch process. Such issue can be avoided by electrocatalytic N2 reduction which however suffers from limited current efficiency and NH3 yield. Herein, we demonstrate ambient NH3 production via electrochemical nitrite (NO2) reduction catalyzed by a CoP nanoarray on titanium mesh (CoP NA/TM). When tested in 0.1 M PBS (pH = 7) containing 500 ppm NO2, such CoP NA/TM is capable of affording a large NH3 yield of 2, 260.7 ± 51.5 μg·h–1·cm–2 and a high Faradaic efficiency of 90.0 ± 2.3% at –0.2 V vs. a reversible hydrogen electrode. Density functional theory calculations reveal that the potential-determining step for NO2 reduction over CoP (112) is *NO2 → *NO2H.

Keywords: density functional theory, electrocatalysis, CoP nanoarray, NO2 reduction reaction, ambient NH3 synthesis

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Acknowledgements

Publication history

Received: 14 February 2021
Revised: 24 April 2021
Accepted: 12 May 2021
Published: 09 June 2021
Issue date: February 2022

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© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22072015) and Shanghai Scientific and Technological Innovation Project (No. 18JC1410604).

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