Elimination of Interlayer Potential Barriers of Chromium Sulfide by Self-Intercalation for Enhanced Hydrogen Evolution Reaction

Meixia Su; Wenda Zhou; Zhenzhen Jiang; Mingyue Chen; Xingfang Luo; Jun He; Cailei Yuan

doi:10.1021/acsami.0c20577

Elimination of Interlayer Potential Barriers of Chromium Sulfide by Self-Intercalation for Enhanced Hydrogen Evolution Reaction

ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13055-13062. doi: 10.1021/acsami.0c20577. Epub 2021 Mar 9.

Authors

Meixia Su¹, Wenda Zhou^{1

2}, Zhenzhen Jiang¹, Mingyue Chen¹, Xingfang Luo¹, Jun He³, Cailei Yuan¹

Affiliations

¹ Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang 330022, Jiangxi, China.
² School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China.
³ Hunan Key Laboratory for Super-Micro Structure and Ultrafast Process, School of Physics and Electronics, Central South University, 932 South Lushan Road, Changsha 410083, Hunan, China.

PMID: 33689265
DOI: 10.1021/acsami.0c20577

Abstract

The van der Waals (vdW) gaps in layered transition-metal dichalcogenides (TMDs) with an interlayer poor charge transport are considered the bottleneck for higher hydrogen evolution reaction (HER) performance of TMDs. Filling the vdW gap of TMDs materials with intercalants is considered a good way to generate new interesting properties. However, postsynthesis intercalation with foreign atoms may bring extra crystalline imperfections and low yields. In this work, to overcome the interlayer potential barriers of TMDs, CrS₂-Cr_1/3-CrS₂ is produced by naturally self-intercalating native Cr_1/3 atom plane into the vdW layered CrS₂. The CrS₂-Cr_1/3-CrS₂ exhibits strong chemical bonds and high electrical conductivity, which can provide excellent HER electrocatalytic performance. Moreover, based on the first-principles calculations and experimental verification, the intercalated Cr atoms exhibit a Gibbs free energy of the adsorbed hydrogen close to zero and could further improve the electrocatalytic HER performance. Our work provides a new view in self-intercalation for electrocatalysis applications.

Keywords: electrocatalysis; hydrogen evolution reaction; interlayer potential barriers; self-intercalation; transition-metal dichalcogenides; van der Waals layered materials.