First principles screening of transition metal single-atom catalysts for nitrogen reduction reaction

被引：30

作者：

Bo, Tingting ^{[1
]}

Cao, Shiqian ^{[1
]}

Mu, Nan ^{[1
]}

Xu, Ruixin ^{[1
]}

Liu, Yanyu ^{[2
]}

Zhou, Wei ^{[1
]}

机构：

[1] Tianjin Univ, Sch Sci, Dept Appl Phys, Tianjin Key Lab Low Dimens Mat Phys & Preparing Te, Tianjin 300072, Peoples R China

[2] Tianjin Normal Univ, Coll Phys & Mat Sci, Tianjin 300387, Peoples R China

来源：

APPLIED SURFACE SCIENCE | 2023年 / 612卷

基金：

中国国家自然科学基金;

关键词：

DFT screening; Single-atom catalyst; -Sb monolayer; Nitrogen reduction reaction; Selectivity; ELECTROCHEMICAL AMMONIA-SYNTHESIS; CLUSTER CATALYST; ELECTROCATALYSTS; MONOLAYERS; ANTIMONENE; IRON; PHOSPHORENE; NANOSHEETS; DYNAMICS; NB;

D O I：

10.1016/j.apsusc.2022.155916

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The discovery of metals as catalytic centers for nitrogen reduction reactions (NRR) has stimulated great enthusiasm for single-atom catalysts. However, the poor activity and low selectivity of available single-atom catalysts (SACs) are far away from the industrial requirement. Through the first principles screening, the doping engineering can effectively regulate the NRR performance of beta-Sb monolayer. Especially, the origin of activated N2 is discovered from the perspective of the electronic structure of the active center. Among the 24 transition metal dopants, Re@Sb showed the best NRR catalytic performance with a low limiting potential. The Re@Sb also could significantly inhibit hydrogen evolution reaction (HER) and achieve a high theoretical Faradaic efficiency of 100%. Our findings not only accelerate discovery of catalysts for ammonia synthesis but also contribute to further elucidate the structure-performance correlations.

引用

页数：12

共 64 条

[1] The melting curve of iron at the pressures of the Earth's core from ab initio calculations [J].