密度泛函理论
单层
共轭体系
催化作用
金属
Atom(片上系统)
材料科学
过渡金属
化学
计算化学
纳米技术
计算机科学
有机化学
聚合物
嵌入式系统
作者
Chun Wang,Xiaocheng Zhou,Yafei Li
出处
期刊:2D materials
[IOP Publishing]
日期:2023-02-10
卷期号:10 (2): 024002-024002
标识
DOI:10.1088/2053-1583/acb784
摘要
Abstract Achieving efficient nitrogen reduction reaction (NRR) under mild conditions is desirable but still challenging due to the lack of high-performance catalysts. Herein, we report the feasibility of a new type of two-dimensional conjugated metal–organic frameworks (cMOFs) featuring dense single-metal-atom sites, namely TM 3 (HAT) 2 monolayers (TM = transition metal from groups 4 to 10, HAT = 1,4,5,8,9,12-hexaazatriphenylene), as NRR catalysts. We construct an efficient four-step screening strategy and identify the W 3 (HAT) 2 monolayer as a candidate with considerable stability, activity, and selectivity based on density functional theory (DFT) computations. The analysis of bonding, integrated-crystal orbital Hamilton population, and Bader charge uncovers the NRR activity origin of the TM 3 (HAT) 2 monolayers and elucidates the structure–performance correlations. Meanwhile, our results show that a simple descriptor ϕ based on the inherent nature of the TM atoms can be applied to accelerate the screening of candidates without explicit DFT calculations. This work highlights a feasible strategy to prescreen and design high-performance cMOF-based electrocatalysts.
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