Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia
Abstract Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3 − adsorption on cathode sur...
| Main Authors: | , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-39366-9 |
| _version_ | 1827916798656249856 |
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| author | Shuo Zhang Jianghua Wu Mengting Zheng Xin Jin Zihan Shen Zhonghua Li Yanjun Wang Quan Wang Xuebin Wang Hui Wei Jiangwei Zhang Peng Wang Shanqing Zhang Liyan Yu Lifeng Dong Qingshan Zhu Huigang Zhang Jun Lu |
| author_facet | Shuo Zhang Jianghua Wu Mengting Zheng Xin Jin Zihan Shen Zhonghua Li Yanjun Wang Quan Wang Xuebin Wang Hui Wei Jiangwei Zhang Peng Wang Shanqing Zhang Liyan Yu Lifeng Dong Qingshan Zhu Huigang Zhang Jun Lu |
| author_sort | Shuo Zhang |
| collection | DOAJ |
| description | Abstract Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3 − adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH3 yield rate of 1.08 mmol h−1 mg−1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO3 − and Fe/Cu promotes the adsorption and discharge of NO3 − anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate reduction and ammonia synthesis. |
| first_indexed | 2024-03-13T03:20:23Z |
| format | Article |
| id | doaj.art-a679d0ef5121435aba24a8b2e5e1c422 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T03:20:23Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-a679d0ef5121435aba24a8b2e5e1c4222023-06-25T11:22:28ZengNature PortfolioNature Communications2041-17232023-06-0114111010.1038/s41467-023-39366-9Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammoniaShuo Zhang0Jianghua Wu1Mengting Zheng2Xin Jin3Zihan Shen4Zhonghua Li5Yanjun Wang6Quan Wang7Xuebin Wang8Hui Wei9Jiangwei Zhang10Peng Wang11Shanqing Zhang12Liyan Yu13Lifeng Dong14Qingshan Zhu15Huigang Zhang16Jun Lu17State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of SciencesNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityCentre for Clean Environment and Energy and Griffith School of Environment, Griffith UniversityNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityState Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of SciencesNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityNational Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityDalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (CAS)National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityCentre for Clean Environment and Energy and Griffith School of Environment, Griffith UniversityCollege of Materials Science and Engineering, Qingdao University of Science and TechnologyCollege of Materials Science and Engineering, Qingdao University of Science and TechnologyState Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of SciencesState Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of SciencesCollege of Chemical and Biological Engineering, Zhejiang UniversityAbstract Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO3 − adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH3 yield rate of 1.08 mmol h−1 mg−1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO3 − and Fe/Cu promotes the adsorption and discharge of NO3 − anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate reduction and ammonia synthesis.https://doi.org/10.1038/s41467-023-39366-9 |
| spellingShingle | Shuo Zhang Jianghua Wu Mengting Zheng Xin Jin Zihan Shen Zhonghua Li Yanjun Wang Quan Wang Xuebin Wang Hui Wei Jiangwei Zhang Peng Wang Shanqing Zhang Liyan Yu Lifeng Dong Qingshan Zhu Huigang Zhang Jun Lu Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia Nature Communications |
| title | Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| title_full | Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| title_fullStr | Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| title_full_unstemmed | Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| title_short | Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| title_sort | fe cu diatomic catalysts for electrochemical nitrate reduction to ammonia |
| url | https://doi.org/10.1038/s41467-023-39366-9 |
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