ALBERT

Description: 〈p〉Publication date: 15 April 2019〈/p〉 〈p〉〈b〉Source:〈/b〉 Applied Surface Science, Volume 473〈/p〉 〈p〉Author(s): Xiaoping Gao, Yanan Zhou, Yujia Tan, Bowen Yang, Zhiwen Cheng, Zhemin Shen, Jinping Jia〈/p〉 〈div xml:lang="en"〉 〈h5〉Abstract〈/h5〉 〈div〉〈p〉The high-efficient electrochemical hydrogen evolution reaction (HER) is a promising pathway to provide clean energy. An electrocatalyst was computer-aided designed with Mo isolated single atoms (Mo-ISA) supported on heteroatom S, N-codoped carbon having excellent HER performance. Here, by performing comprehensive density functional theory (DFT) computations, we investigated the influence of the N dopent concentration and the sites of S atom doping on the HER performance. Our computed results demonstrate that the Mo-ISA/N1C and Mo-ISA/S〈sub〉6〈/sub〉N1C catalysts possess good stability and high HER reactivity. Moreover, the interactions between hydrogen and the Mo atoms could be controlled by the N dopent concentration on carbon support, and the Mo-ISA/N1C catalyst showed best HER reactivity. In particular, the S atom was introduced into Mo-ISA/N1C at the S〈sub〉6〈/sub〉 site showing an enhanced HER performance due to the competitive effect of the S-induced tensile strain and charge transfer. Our DFT computations open up new opportunities for application of S, N-codoped Mo-based high-efficient catalysts for HER.〈/p〉〈/div〉 〈/div〉 〈div xml:lang="en"〉 〈h5〉Graphical abstract〈/h5〉 〈div〉 〈p〉An efficient S, N-codoped carbon supported isolated single Mo atoms catalyst is computer-aided designed, and shows excellent HER performance.〈/p〉 〈p〉〈figure〉〈img src="https://ars.els-cdn.com/content/image/1-s2.0-S0169433218335517-ga1.jpg" width="306" alt="Graphical abstract for this article" title=""〉〈/figure〉〈/p〉 〈/div〉 〈/div〉