Su Meixia, Zhou Wenda, Jiang Zhenzhen, Chen Mingyue, Luo Xingfang, He Jun, Yuan Cailei
Jiangxi Key Laboratory of Nanomaterials and Sensors, School of Physics, Communication and Electronics, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang 330022, Jiangxi, China.
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China.
ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13055-13062. doi: 10.1021/acsami.0c20577. Epub 2021 Mar 9.
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, CrS-Cr-CrS is produced by naturally self-intercalating native Cr atom plane into the vdW layered CrS. The CrS-Cr-CrS 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.
层间电荷传输较差的层状过渡金属二硫属化物（TMDs）中的范德华（vdW）间隙被认为是TMDs析氢反应（HER）性能提升的瓶颈。用插层剂填充TMDs材料的vdW间隙被认为是产生新的有趣特性的好方法。然而，用外来原子进行合成后插层可能会带来额外的晶体缺陷和低产率。在这项工作中，为了克服TMDs的层间势垒，通过将天然Cr原子平面自然自插层到vdW层状CrS中制备了CrS-Cr-CrS。CrS-Cr-CrS表现出强化学键和高电导率，能够提供优异的HER电催化性能。此外，基于第一性原理计算和实验验证，插层的Cr原子表现出接近零的吸附氢吉布斯自由能，并能进一步提高电催化HER性能。我们的工作为电催化应用中的自插层提供了新的视角。
