Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect
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<sup>+</sup> 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<sup>+</sup> ions, as indicated by the distance of K<sup>+</sup> 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 mg<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>) and well-maintained the Faradaic efficiency for over 120 h under ampere-level reduction.
Authors
- Peng Gao (ORCID: https://orcid.org/0000-0001-8938-6701)
- Qianyu Liu (ORCID: https://orcid.org/0000-0002-2660-7287)
- Jie‐Sheng Chen (ORCID: https://orcid.org/0000-0003-1233-7746)
- Shi‐Nan Zhang (ORCID: https://orcid.org/0000-0001-8138-3610)
- Bing‐Liang Leng (ORCID: https://orcid.org/0000-0002-9738-8181)
- Xin‐Hao Li (ORCID: https://orcid.org/0000-0003-1643-4631)
- Zhao Zhang (ORCID: https://orcid.org/0009-0006-0212-9168)
Institutions
- Shanghai Jiao Tong University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-12-30
- DOI
- https://doi.org/10.1038/s41467-024-55230-w
- Citations
- 56
- Primary Topic
- Ammonia Synthesis and Nitrogen Reduction
- Type
- article
- Field-Weighted Citation Impact
- 5.99
Funders
- National Natural Science Foundation of China
- Science and Technology Commission of Shanghai Municipality
- Shanghai Shuguang Program