Citation: Yahui Li, Quanchen Feng, Krisztina László, Ying Wang. High-throughput screening of high C/N-ratio homonuclear dual-atom catalysts for electrochemical reduction of nitrate to ammonia[J]. Chinese Chemical Letters, ;2026, 37(3): 111536. doi: 10.1016/j.cclet.2025.111536 shu

High-throughput screening of high C/N-ratio homonuclear dual-atom catalysts for electrochemical reduction of nitrate to ammonia

a.
State Key Laboratory of Water Pollution Control and Green Resource Recycling, Shanghai Institute of Pollution Control and Ecological Security, School of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
b.
Department of Physical Chemistry and Materials Science, Faculty of Chemical Technology and Biotechnology, Budapest University of Technology and Economics, Budapest 1111, Hungary

yingwang@tongji.edu.cn

Received Date: 21 December 2024
Revised Date: 30 April 2025
Accepted Date: 2 July 2025
Available Online: 3 July 2025

Figures(5)

To deal with the problem of NO₃⁻ enrichment in water environment, electrochemical catalysis of nitrate reduction reaction (NO₃RR) provides a possibility. However, this catalytic process requires efficient and highly selective NO₃RR electrocatalysts to catalyze NO₃⁻ conversion. Consequently, the objective of this work is to search highly active NO₃RR electrocatalysts by employing an efficient screening strategy using density functional theory methods. The catalytic activity is assessed by calculating limiting potential U_L(NO₃RR) and U_L(HER). The research results indicate that Os₂_C₁₉N₃ not only has excellent catalytic activity (U_L(NO₃RR) = −0.15 V), but also can effectively avoid the occurrence of competitive hydrogen evolution reaction. The NO₃RR process of Os₂_C₁₉N₃ is * + NO₃⁻ → ^*NO₃ → ^*NO₃H → NO₂ → ^*NO₂H → ^*NO → ^*NOH → ^*N → ^*NH → ^*NH₂ → ^*NH₃ → * + NH₃. When Os₂_C₁₉N₃ is in the condition of DFT-Sol, DFT-D, and DFT-D-Sol, the NO₃RR process is * + NO₃⁻ → ^*NO₃ → ^*NO₃H → NO₂ → ^*NO₂H → ^*NO → ^*NOH → ^*NHOH → ^*NH₂OH → ^*NH₂ → ^*NH₃ → * + NH₃, and the U_L(NO₃RR) values are −0.06, −0.15, and −0.06 V, respectively. This research may offer potential reference values for the development of innovative NO₃RR catalysts and the synthesis of NH₃.
- Homonuclear dual-atom catalysts,
- Electrocatalysis,
- Nitrate reduction reaction,
- Hydrogen evolution reaction,
- Density functional theory
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