期刊
ACS CATALYSIS
卷 -, 期 -, 页码 7655-7663出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01293
关键词
ENRR; Mo/BCN; single-atom electrocatalyst; density functional theory; pH-universal
资金
- National Natural Science Foundation of China [U1808210]
- Dalian Science and Technology Innovation Fund [2020JJ26GX044]
In this study, B/N codoped porous carbon nanotube-supported single Mo site catalysts were designed and synthesized for efficient electrochemical N-2 reduction reaction. The catalyst exhibited high catalytic activity and faradaic efficiency, making it a promising candidate for artificial ammonia synthesis.
Electrochemical N-2 reduction reaction (ENRR) at ambient temperature is a futuristic method for the artificial synthesis of ammonia, but it is still not efficient enough to be applied on a large scale. Inspired by the molybdenum-containing nitrogen-fixing enzymes of rhizobia in nature, single Mo sites are predicted to serve as an effective catalyst for ENRR. Herein, B/N codoped porous carbon nanotube-supported single Mo site catalysts (Mo/BCN) were rationally designed and synthesized. Mo/BCN exhibits the highest catalytic activity toward N-2 fixation to NH3 with a yield rate of 37.67 mu g h(-1) mg(cat)(-1) and a faradaic efficiency of 13.27% in 0.1 M KOH, which is better than those of nonprecious metal electrocatalysts. Density functional theory and extended X-ray absorption fine structure analysis indicated that single-atom Mo sites could be anchored on BCN nanotubes and act as sufficient active sites for nitrogen reduction. The present work may provide a theoretical and experimental strategy for developing efficient single-atom catalysts for ENRR.
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