Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect
Abstract Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particul...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-12-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55230-w |
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| author | Shi-Nan Zhang Peng Gao Qian-Yu Liu Zhao Zhang Bing-Liang Leng Jie-Sheng Chen Xin-Hao Li |
| author_facet | Shi-Nan Zhang Peng Gao Qian-Yu Liu Zhao Zhang Bing-Liang Leng Jie-Sheng Chen Xin-Hao Li |
| author_sort | Shi-Nan Zhang |
| collection | DOAJ |
| description | Abstract Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particularly in pure nitrate solutions. Herein, we present the application of electron deficiency of Ru metals to boost the repelling effect of counter K+ ions via the electric-field-dependent synergy of interfacial water and cations, and thus largely promote nitrate reduction reaction with a high yield and well-maintained Faradaic efficiency under ampere-level current density. The pronounced electron deficiency of Ru metals boosts the repelling effect on hydrated K+ ions, as indicated by the distance of K+ ions to catalyst surface, which can loosen the water layer to depress hydrogen evolution and accelerate nitrate conversion. Consequently, the optimized electrode loaded with electron-deficient Ru atomic layers can directly produce 0.26 M ammonia solution in pure nitrate solution in 6 h, providing a high yield (74.8 mg mgcat –1 h–1) and well-maintained the Faradaic efficiency for over 120 h under ampere-level reduction. |
| format | Article |
| id | doaj-art-33f364996ebf4bc99bcfc81c84940d5c |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-33f364996ebf4bc99bcfc81c84940d5c2025-01-05T12:36:18ZengNature PortfolioNature Communications2041-17232024-12-0115111210.1038/s41467-024-55230-wAmpere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effectShi-Nan Zhang0Peng Gao1Qian-Yu Liu2Zhao Zhang3Bing-Liang Leng4Jie-Sheng Chen5Xin-Hao Li6School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong UniversityAbstract Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particularly in pure nitrate solutions. Herein, we present the application of electron deficiency of Ru metals to boost the repelling effect of counter K+ ions via the electric-field-dependent synergy of interfacial water and cations, and thus largely promote nitrate reduction reaction with a high yield and well-maintained Faradaic efficiency under ampere-level current density. The pronounced electron deficiency of Ru metals boosts the repelling effect on hydrated K+ ions, as indicated by the distance of K+ ions to catalyst surface, which can loosen the water layer to depress hydrogen evolution and accelerate nitrate conversion. Consequently, the optimized electrode loaded with electron-deficient Ru atomic layers can directly produce 0.26 M ammonia solution in pure nitrate solution in 6 h, providing a high yield (74.8 mg mgcat –1 h–1) and well-maintained the Faradaic efficiency for over 120 h under ampere-level reduction.https://doi.org/10.1038/s41467-024-55230-w |
| spellingShingle | Shi-Nan Zhang Peng Gao Qian-Yu Liu Zhao Zhang Bing-Liang Leng Jie-Sheng Chen Xin-Hao Li Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect Nature Communications |
| title | Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect |
| title_full | Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect |
| title_fullStr | Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect |
| title_full_unstemmed | Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect |
| title_short | Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect |
| title_sort | ampere level reduction of pure nitrate by electron deficient ru with k ions repelling effect |
| url | https://doi.org/10.1038/s41467-024-55230-w |
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