High-throughput screening of N-doped curved graphene-loaded transition metal single-atom catalysts for nitrogen reduction reaction

• Published in: Applied surface science 2024-06, Vol.658, p.159858, Article 159858
• Main Authors: Wang, Jingang, Li, Ning, Jiang, Yongjian, Sheng, Hao, Sun, Mengtao
• Format: Article
• Language: English
• ISSN: 0169-4332; 1873-5584
• DOI: 10.1016/j.apsusc.2024.159858

[Display omitted] •A graphene-loaded transition metal single-atom catalyst doped with nitrogen atoms was designed.•Five catalysts with excellent NRR catalytic performance were screened from 406 catalysts, with the lowest limiting potential of 0.31 V.•Screening strategy: ① The adsorption energy of N2 ＜ 0.5 eV; ② The free energy barriers for the first and last hydrogenation reactions ＜ 0.4 eV; ③ The free energy of desorption of NH3 ＜1 eV; ④ Better NRR selectivity than HER. Nitrogen reduction reaction (NRR) is necessary as an environmentally friendly and sustainable method for producing NH3 in the context of the energy crisis and increasing environmental concerns. Efficient catalysts play an important role in the NRR reaction. In this work, a high-curvature tetracoordinate transition metal (TM) nitrogen-doped graphene single-atom catalyst was designed and five candidate catalysts with excellent performances were selected from 406 models through a combination of high-throughput screening and density functional theory calculations. Using seven different coordination types MC4, MC3N1, MC2N2-1, MC2N2-2, MC2N2-3, MC1N3 and MN4, of which VN4 (side-on) with four N-atom coordination has the lowest limiting potential of 0.31 V and the competing Hydrogen Evolution Reaction (HER) was suppressed. This work provides guidance for the development of efficient NRR catalysts.