Hydrogen Evolution Reaction at Anion Vacancy of Two-Dimensional Transition-Metal Dichalcogenides: Ab Initio Computational Screening

被引：117

作者：

Lee, Joohee ^{[1
,2
]}

Kang, Sungwoo ^{[1
,2
]}

Yim, Kanghoon ^{[1
,2
,4
]}

Kim, Kye Yeop ^{[1
,2
,5
]}

Jang, Ho Won ^{[1
,2
]}

Kang, Youngho ^{[3
]}

Han, Seungwu ^{[1
,2
]}

机构：

[1] Seoul Natl Univ, Dept Mat Sci & Engn, Seoul 08826, South Korea

[2] Seoul Natl Univ, Res Inst Adv Mat, Seoul 08826, South Korea

[3] Korea Inst Mat Sci, Mat Modeling & Characterizat Dept, Chang Won 51508, South Korea

[4] Korea Inst Energy Res, 152 Gajeong Ro, Daejeon 34129, South Korea

[5] LGE Yangjae R&D Campus,38 Baumoe Ro, Seoul 06763, South Korea

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2018年 / 9卷 / 08期

关键词：

CATALYTIC-ACTIVITY; MOS2; WS2; MX2; ELECTROCATALYST; NANOSHEETS; EFFICIENT; SUPPORT; PHASE; SE;

D O I：

10.1021/acs.jpclett.8b00712

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 catalytic activity for the hydrogen evolution reaction (HER) at the anion vacancy of 40 2D transition-metal dichalcogenides (TMDs) is investigated using the hydrogen adsorption free energy (AGH) as the activity descriptor. While vacancy-free basal planes are mostly inactive, anion vacancy makes the hydrogen bonding stronger than clean basal planes, promoting the HER performance of many TMDs. We find that ZrSe2 and ZrTe2 have similar AGH as Pt, the best HER catalyst, at low vacancy density. AGH depends significantly on the vacancy density, which could be exploited as a tuning parameter. At proper vacancy densities, MoS2, MoSe2, MoTe2, ReSe2, ReTe2, WSe2, IrTe2, and HfTe2 are expected to show the optimal HER activity. The detailed analysis of electronic structure and the multiple linear regression results identifies the vacancy formation energy and band-edge positions as key parameters correlating with AGH at anion vacancy of TMDs.

引用

页码：2049 / 2055

页数：13

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