Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2
Abstract Nitrate (NO3 ‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3 ‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3 ‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficien...
| Main Authors: | , , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-45534-2 |
| _version_ | 1797274159164686336 |
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| author | Wanru Liao Jun Wang Ganghai Ni Kang Liu Changxu Liu Shanyong Chen Qiyou Wang Yingkang Chen Tao Luo Xiqing Wang Yanqiu Wang Wenzhang Li Ting-Shan Chan Chao Ma Hongmei Li Ying Liang Weizhen Liu Junwei Fu Beidou Xi Min Liu |
| author_facet | Wanru Liao Jun Wang Ganghai Ni Kang Liu Changxu Liu Shanyong Chen Qiyou Wang Yingkang Chen Tao Luo Xiqing Wang Yanqiu Wang Wenzhang Li Ting-Shan Chan Chao Ma Hongmei Li Ying Liang Weizhen Liu Junwei Fu Beidou Xi Min Liu |
| author_sort | Wanru Liao |
| collection | DOAJ |
| description | Abstract Nitrate (NO3 ‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3 ‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3 ‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3 ‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm–2 and enables an over 99% NO3 –-to-NH3 conversion efficiency. We also convert NO3 ‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3 ‒-to-NH3 conversion. |
| first_indexed | 2024-03-07T14:54:23Z |
| format | Article |
| id | doaj.art-514888f4cdea454594453232136cf88d |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-07T14:54:23Z |
| publishDate | 2024-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-514888f4cdea454594453232136cf88d2024-03-05T19:31:24ZengNature PortfolioNature Communications2041-17232024-02-0115111210.1038/s41467-024-45534-2Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2Wanru Liao0Jun Wang1Ganghai Ni2Kang Liu3Changxu Liu4Shanyong Chen5Qiyou Wang6Yingkang Chen7Tao Luo8Xiqing Wang9Yanqiu Wang10Wenzhang Li11Ting-Shan Chan12Chao Ma13Hongmei Li14Ying Liang15Weizhen Liu16Junwei Fu17Beidou Xi18Min Liu19Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityCentre for Metamaterial Research & Innovation, Department of Engineering, University of ExeterSchool of Chemistry and Chemical Engineering, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversitySchool of Chemistry and Chemical Engineering, Central South UniversitySchool of Chemistry and Chemical Engineering, Central South UniversityNational Synchrotron Radiation Research CenterCollege of Materials Science and Engineering, Hunan UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityCollege of Food Science and Engineering, Central South University of Forestry and TechnologySchool of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of TechnologyHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityState Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental SciencesHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityAbstract Nitrate (NO3 ‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3 ‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3 ‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3 ‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm–2 and enables an over 99% NO3 –-to-NH3 conversion efficiency. We also convert NO3 ‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3 ‒-to-NH3 conversion.https://doi.org/10.1038/s41467-024-45534-2 |
| spellingShingle | Wanru Liao Jun Wang Ganghai Ni Kang Liu Changxu Liu Shanyong Chen Qiyou Wang Yingkang Chen Tao Luo Xiqing Wang Yanqiu Wang Wenzhang Li Ting-Shan Chan Chao Ma Hongmei Li Ying Liang Weizhen Liu Junwei Fu Beidou Xi Min Liu Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 Nature Communications |
| title | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 |
| title_full | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 |
| title_fullStr | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 |
| title_full_unstemmed | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 |
| title_short | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 |
| title_sort | sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 a cm 2 |
| url | https://doi.org/10.1038/s41467-024-45534-2 |
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