Computational screening of pyrazine-based graphene-supported transition metals as single-atom catalysts for the nitrogen reduction reaction.
Min ZhangCaijuan XiaLianbi LiAnxiang WangDezhong CaoBaiyu ZhangQing-Long FangXumei ZhaoPublished in: Dalton transactions (Cambridge, England : 2003) (2024)
Electrochemical synthesis of NH 3 from N 2 utilizing single-atom catalysts (SACs) is a promising strategy for industrial nitrogen fixation and chemical raw material production. In this work, single transition metals (TMs) anchored on pyrazine-based graphene (TM@py-GY) are systematically studied to screen potential electrocatalysts for the nitrogen reduction reaction (NRR) using first-principles calculations. Particularly, the descriptor φ related to electronegativity and valence electron number is selected to clarify the trend of NRR activity, realizing a fast-scan/estimation among various candidates. After a four-step screening process, W I @py-GY and Mo II @py-GY SACs are screened with good structural stability, high selectivity, and high activity. Meanwhile, the thermodynamic stability of W I @py-GY and Mo II @py-GY SACs is demonstrated to ensure their feasibility in real experimental conditions. Furthermore, electronic properties are also examined in detail to analyze activity origin. This work not only provides an effective and reliable method for screening electrochemical NRR catalysts with excellent performance but also provides guidance for the rational design of SACs.
Keyphrases
- electron transfer
- molecular dynamics
- highly efficient
- human health
- ionic liquid
- computed tomography
- minimally invasive
- metal organic framework
- heavy metals
- health risk
- density functional theory
- high resolution
- high throughput
- risk assessment
- wastewater treatment
- molecular dynamics simulations
- carbon nanotubes
- single cell
- walled carbon nanotubes
- drinking water
- solid state