Elimination of Interlayer Potential Barriers of Chromium Sulfide by Self-Intercalation for Enhanced Hydrogen Evolution Reaction
Elimination of Interlayer Potential Barriers of Chromium Sulfide by Self-Intercalation for Enhanced Hydrogen Evolution Reaction
复制标题
自插层消除硫化铬层间势垒增强析氢反应
DOI：
10.1021/acsami.0c20577
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发表时间：
2021
影响因子：
9.5
通讯作者：
Cailei Yuan
中科院分区：
文献类型：
--
作者：
Meixia Su;Wenda Zhou;Zhenzhen Jiang;Mingyue Chen;Xingfang Luo;Jun He;Cailei Yuan
层状过渡金属二卤化物(TMDs)中的范德华(VDW)能隙具有较差的电荷输运能力，是提高TMDs析氢性能的瓶颈。用插层剂填充TMDS材料的VDW空隙被认为是产生新的有趣性质的好方法。然而，合成后与外来原子的插层可能会带来额外的结晶缺陷和低的产率。在这项工作中，为了克服TMD的层间势垒，通过自然地将自然的Cr1/3原子平面插入到VDW层状的CrS2中，产生了CrS2-Cr1/3-CrS2。CrS2-Cr1/3-CrS2具有较强的化学键和较高的电导率，可提供优异的HER电催化性能。此外，基于第一性原理计算和实验验证，插层铬原子的吉布斯自由能接近于零，可以进一步提高电催化性能。我们的工作为自插层电催化应用提供了一个新的视角。
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–CrS2is produced by naturally self-intercalating native Cr1/3atom plane into the vdW layered CrS2. The CrS2–Cr1/3–CrS2exhibits 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.