Nickel bis(dithiolene) complexes for electrocatalytic hydrogen evolution: A computational study

Zhang, Zisheng3; Yang, Tilong3; Qin, Peng1,2; Dang, Li1,2,3

2018-06

10.1016/j.jorganchem.2018.03.007

JOURNAL OF ORGANOMETALLIC CHEMISTRY   影响因子和分区

0022-328X

1872-8561

The substituent effect of dithiolene ligand on electrocatalytic activity of Ni bis(dithiolene) towards hydrogen evolution reaction (HER) are thoroughly explored with computational methods. A series of differently substituted dithiolene ligands are compared and evaluated. These computational results indicate that adding electron-withdrawing groups on the ligand or enlarging the conjugate Pi system of the ligand can greatly reduce the reduction potentials, while tuning the electronic structure of the non-innocent framework can optimize the geometry of dihydrogen species to achieve lower energy barrier for H-2 elimination. This study may benefit the deep understanding of the electrocatalyzed HER mechanism and give inspirations on the design of efficient nickel bis(dithiolene) electrocatalysts with low overpotential and improved kinetics. (C) 2018 Published by Elsevier B.V.

Reaction mechanism DFT calculation Non-innocent complex Hydrogen evolution reaction Ligand effects

SCI ; EI

英语

第一 ; 通讯

National Natural Science Foundation of China[21573102]

Chemistry

Chemistry, Inorganic & Nuclear ; Chemistry, Organic

WOS:000432598600019

ELSEVIER SCIENCE SA

20181304949549

Design for testability ; Electrocatalysis ; Electrocatalysts ; Electronic structure ; Hydrogen ; Ligands

Computer Applications:723.5 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804

CHEMISTRY

Web of Science

1.Shantou Univ, Dept Chem, Shantou 515063, Guangdong, Peoples R China
2.Shantou Univ, Key Lab Preparat & Applicat Ordered Struct Mat Gu, Shantou 515063, Guangdong, Peoples R China
3.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Zhang, Zisheng,Yang, Tilong,Qin, Peng,et al. Nickel bis(dithiolene) complexes for electrocatalytic hydrogen evolution: A computational study[J]. JOURNAL OF ORGANOMETALLIC CHEMISTRY,2018,864:143-147.

Zhang, Zisheng,Yang, Tilong,Qin, Peng,&Dang, Li.(2018).Nickel bis(dithiolene) complexes for electrocatalytic hydrogen evolution: A computational study.JOURNAL OF ORGANOMETALLIC CHEMISTRY,864,143-147.

Zhang, Zisheng,et al."Nickel bis(dithiolene) complexes for electrocatalytic hydrogen evolution: A computational study".JOURNAL OF ORGANOMETALLIC CHEMISTRY 864(2018):143-147.