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.

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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

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article

Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect

Peng Gao, Qianyu Liu, Jie‐Sheng Chen, Shi‐Nan Zhang et al.
56 citations
Nature Communications
Ammonia Synthesis and Nitrogen Reduction
5.99
article

Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect

Peng Gao, Qianyu Liu, Jie‐Sheng Chen, Shi‐Nan Zhang, Bing‐Liang Leng, Xin‐Hao Li, Zhao Zhang
article en
56 citations

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<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.

Nature CommunicationsVol. 15(1)
Shanghai Jiao Tong University (CN)
National Natural Science Foundation of China, Science and Technology Commission of Shanghai Municipality, Shanghai Shuguang Program
Responsible consumption and production
Openalex Percentile: Top 3%
Ammonia Synthesis and Nitrogen Reduction
5.99
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Ampere-level reduction of pure nitrate by electron-deficient Ru with K+ ions repelling effect — Peng Gao, Qianyu Liu, et al. · Nature Communications (2024) | TGRS Research Map | TGRS