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-Cr1/3-CrS2 is produced by naturally self-intercalating native Cr1/3 atom plane into the vdW layered CrS2. The CrS2-Cr1/3-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.
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