Citation: Anni Wu, Chengyi Hong, Hu Zheng, Wei Teng. Multi-site synergistic relay electrocatalysis with high-entropy nanoalloys for effective nitrate reduction to ammonia[J]. Chinese Chemical Letters, ;2025, 36(12): 111066. doi: 10.1016/j.cclet.2025.111066 shu

Multi-site synergistic relay electrocatalysis with high-entropy nanoalloys for effective nitrate reduction to ammonia

Anni Wu ^{a, b} ,
Chengyi Hong ^c ,
Hu Zheng ^{a, d} ,
Wei Teng ^{b, *,}

a.
Department of Geotechnical Engineering, College of Civil Engineering, Tongji University, Shanghai 200092, China
b.
State Key Laboratory for Pollution Control, School of Environmental Science and Engineering, Shanghai Institute of Pollution Control and Ecological Security, China Key Laboratory of Urban Water Supply, Water Saving and Water Environment Governance in the Yangtze River Delta of Ministry of Water Resources, Tongji University, Shanghai 200092, China
c.
Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
d.
Key Laboratory of Geotechnical and Underground Engineering of the Ministry of Education, State Key Laboratory of Disaster Reduction in Civil Engineering, Tongji University, Shanghai 200092, China

wteng@tongji.edu.cn

Received Date: 26 December 2024
Revised Date: 6 March 2025
Accepted Date: 10 March 2025
Available Online: 12 March 2025

Figures(5)

Electrocatalytic reduction of nitrate to ammonia offers an environmentally friendly and sustainable approach for ammonia production, but it involves a multi-step reaction process with complex intermediates, and still faces the challenge of high activity and high selectivity. Herein, a high-entropy nanoalloy was synthesized via high-temperature annealing of metal salt with dopamine as a carbon source for electrocatalytic reduction of nitrate to ammonia. The FeCoNiCuRu_1.5/C catalyst displays a conversion rate of 90.2% and an ammonia selectivity of 92.2% at -0.74 V (vs. RHE), significantly surpassing the performance of low-entropy alloys such as FeCo/C by 1.5–2 times. Moreover, FeCoNiCuRu_1.5/C maintains a consistent nitrate conversion rate of about 90.0% after 120 h of continuous operation (10 cycles), indicating high stability. The superior performance of FeCoNiCuRu_1.5/C can be attributed to the synergetic relay catalysis among Fe, Co, Ni, Cu, and Ru sites. This synergy enhances nitrate adsorption due to the optimized electronic structure of multiple active sites, which facilitates the nitrate reduction to intermediates. Subsequently, the effective active hydrogen produced at the Ru site, in conjunction with adjustments at other metal sites, promotes the selective transformation of the intermediates into ammonia. This work not only highlights the efficacy of synergetic relay electrocatalysis but also opens new avenues for developing highly efficient multi-site catalysts.
- Electrocatalysis,
- High-entropy alloy,
- Nitrate reduction,
- Ammonia,
- Active hydrogen
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