Efficient nitric oxide reduction to ammonia on a metal-free electrocatalyst

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2021-03, Vol.9 (9), p.5434-5441
• Main Authors: Wu, Qian, Wang, Hao, Shen, Shiying, Huang, Baibiao, Dai, Ying, Ma, Yandong
• Format: Article
• Language: English
• Subjects: Ammonia; Catalytic activity; Chemical reduction; Electrocatalysts; Electrochemistry; First principles; Hybridization; Nitric oxide; Selectivity; Synthesis
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d0ta11209g

NH 3 synthesis and NO removal are two of the most attractive and challenging processes in electrochemistry. Current research efforts mainly focus on them separately, while the direct electrochemical reduction of NO to NH 3 has been less explored. Herein, based on first-principles calculations, we propose a metal-free electrocatalyst, namely, P atom doped single-layer C 2 N, as a promising candidate system for achieving the direct electroreduction of NO to NH 3 . Particularly, double P doped C 2 N (2P@C 2 N) exhibits excellent catalytic activity and high selectivity, which correlates with the sp 3 hybridization of the P atom. Moreover, our microkinetic modeling analysis shows that the turnover frequency of NO reduction to NH 3 on 2P@C 2 N is as large as 8.9 × 10 5 per s per site at 400 K, suggesting that it exhibits an ultra-fast reaction rate. Our study provides not only the first metal-free electrocatalyst for NO removal, but also an effective alternative avenue for ammonia synthesis. P@C 2 N monolayer is predicted as a metal-free electrocatalyst for NO removal, and we propose that the NORR could be an effective alternative avenue for ammonia synthesis.