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

Shi-Nan Zhang, Peng Gao, Qian-Yu Liu, Zhao Zhang, Bing-Liang Leng, Jie-Sheng Chen and Xin-Hao Li ()
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Shi-Nan Zhang: Shanghai Jiao Tong University
Peng Gao: Shanghai Jiao Tong University
Qian-Yu Liu: Shanghai Jiao Tong University
Zhao Zhang: Shanghai Jiao Tong University
Bing-Liang Leng: Shanghai Jiao Tong University
Jie-Sheng Chen: Shanghai Jiao Tong University
Xin-Hao Li: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-55230-w

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