Constructing Ru single-atomic sites through potential-induced self-reconstruction to accelerate electrocatalytic nitrate reduction for ammonia production
CHEMICAL ENGINEERING JOURNAL(2024)
摘要
Conversion of NO3--to-NH3 via the electrocatalytic nitrate reduction reaction (NO3-RR) is an emerging strategy for ammonia production and storage of "green hydrogen", but is limited by the dissatisfactory activity and selectivity. In this study, we discovered that cobalt carbonate hydroxide (Co-2(OH)(2)CO3) underwent a potential-induced self-reconstruction to cobalt hydroxide (Co(OH)(2)) during NO3-RR. The incorporation of Ru into Co-2(OH)(2)CO3 expedited the aforementioned self-reconstruction process and resulted in the formation of Ru single-atomic sites (Ru SASs) anchored on Co(OH)(2) nanosheets. This structure is reported as a highly efficient electrocatalyst for NO3--to-NH3 conversion and exhibits exceptional electrochemical performance in zinc-NO3- batteries. Theoretical analysis revealed that the conversion of NO3--to-NH3 occurred on Ru SASs through an N-end pathway with *NO as a characteristic intermediate. Furthermore, Ru SASs facilitated the thermodynamic-determining step of *NH2-to-*NH3, thus promoting the overall NO3--to-NH3 conversion process.
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关键词
Nitrate reduction reaction,Ammonia,Single atomic catalysts,Self-reconstruction
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