密度泛函理论
催化作用
过电位
材料科学
磷烯
过渡金属
兴奋剂
选择性
氮气
无机化学
化学物理
石墨烯
纳米技术
计算化学
物理化学
化学
光电子学
电化学
电极
生物化学
有机化学
作者
Xin Liu,Chenyin Li,F. Xu,Guohong Fan,Hong Xu
出处
期刊:Nanotechnology
[IOP Publishing]
日期:2022-03-23
卷期号:33 (24): 245401-245401
被引量:13
标识
DOI:10.1088/1361-6528/ac5929
摘要
Ammonia (NH3) is an essential resource in human production and living activities, and its demand has been rising in recent years. The catalytic synthesis of NH3from N2under mild conditions, inspired by biological nitrogen fixation, has piqued the interest of researchers. In this paper, density functional theory (DFT) calculations were used to investigate the catalytic activity, mechanism, and selectivity of the TM embedded nitrogen-doped phosphorene as high-performance nitrogen reduction reaction (NRR) electrocatalysts in depth. The results show that Nb- and Mo-doped catalysts present excellent catalytic performance, with low limiting potentials of -0.41 and -0.18 V, respectively. The Mo-N3-BP catalyst, for example, not only has an extremely low overpotential (-0.02 V), but also presents superior selectivity to effectively inhibit the HER competition reaction. A deeper look into the catalytic mechanism reveals a volcano relationship between the d-band center and the catalytic activity (Mo and Nb are located near the peak of the volcano-type curve). The d-band center and charge of the metal center can be regarded as effective descriptors for NRR activity on TM embedded nitrogen-doped phosphorene electrocatalysts, which hope to serve as a guiding principle for the design of high performance NRR single-atom catalyst in the future.
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