Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations

Abstract Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array e...

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Main Authors: Bocheng Zhang, Zechuan Dai, Yanxu Chen, Mingyu Cheng, Huaikun Zhang, Pingyi Feng, Buqi Ke, Yangyang Zhang, Genqiang Zhang
Format: Article
Language:English
Published: Nature Portfolio 2024-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-47025-w
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author Bocheng Zhang
Zechuan Dai
Yanxu Chen
Mingyu Cheng
Huaikun Zhang
Pingyi Feng
Buqi Ke
Yangyang Zhang
Genqiang Zhang
author_facet Bocheng Zhang
Zechuan Dai
Yanxu Chen
Mingyu Cheng
Huaikun Zhang
Pingyi Feng
Buqi Ke
Yangyang Zhang
Genqiang Zhang
author_sort Bocheng Zhang
collection DOAJ
description Abstract Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm−2 across wide nitrate concentrations (1–100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm−2 at −1.4 V with 99.9% ammonia selectivity and 99.9% nitrate conversion with 100 h stability, demonstrating outstanding practicability.
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spelling doaj.art-340eca74f8634086aced7adb9a6890732024-04-07T11:23:41ZengNature PortfolioNature Communications2041-17232024-04-0115111410.1038/s41467-024-47025-wDefect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrationsBocheng Zhang0Zechuan Dai1Yanxu Chen2Mingyu Cheng3Huaikun Zhang4Pingyi Feng5Buqi Ke6Yangyang Zhang7Genqiang Zhang8Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaHefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of ChinaAbstract Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm−2 across wide nitrate concentrations (1–100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm−2 at −1.4 V with 99.9% ammonia selectivity and 99.9% nitrate conversion with 100 h stability, demonstrating outstanding practicability.https://doi.org/10.1038/s41467-024-47025-w
spellingShingle Bocheng Zhang
Zechuan Dai
Yanxu Chen
Mingyu Cheng
Huaikun Zhang
Pingyi Feng
Buqi Ke
Yangyang Zhang
Genqiang Zhang
Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
Nature Communications
title Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
title_full Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
title_fullStr Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
title_full_unstemmed Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
title_short Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
title_sort defect induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
url https://doi.org/10.1038/s41467-024-47025-w
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