Rational design of freestanding MoS2 monolayers for hydrogen evolution reaction
Rational design of freestanding MoS2 monolayers for hydrogen evolution reaction
复制标题
用于析氢反应的独立式MoS2单分子层的合理设计
DOI：
10.1016/j.nanoen.2017.07.021
复制
发表时间：
2017-09-01
期刊：
影响因子：
17.6
通讯作者：
Ye, Jinhua
中科院分区：
文献类型：
--
作者：
Hai, Xiao;Zhou, Wei;Ye, Jinhua
二硫化钼（MoS 2）是一种有前途的非贵金属析氢反应催化剂，引起了人们的广泛兴趣，但目前还缺乏有效的方法来提高其利用率，特别是在无支撑的2 H-MoS 2基面上。我们报告了一个合理的设计独立的2 H-MoS 2单层，以通过结合结晶工程和钴取代来最大化HER的协同活性。电化学测量和密度泛函理论计算表明，在单层2 H-MoS 2的结晶度工程和钴取代的组合，不仅可以引入大量的缺陷，作为新的活性位点，但也激活和利用的基面，这是负责大大增强HER活性相比，独立的结晶度工程或钴取代。令人印象深刻的是，当与用于光催化析氢的光收集器硫化镉集成时，协同效应还促进了单层2 H-MoS 2的优异助催化性能，甚至高于铂（Pt）。这项研究可能为设计更有效的MoS 2基和其他具有增强HER性能的层状材料提供新的途径。
Molybdenum disulfide (MoS2) presents a promising nonprecious catalyst for hydrogen evolution reaction (HER) that has attracted extensive interest, but it still lacks an effective way to advance the utilization, in particular the basal plane of freestanding 2H-MoS2 for HER. Herein, we report a rational design of freestanding 2H-MoS2 monolayers to maximize the synergistic activity for HER by combining crystallinity engineering and cobalt substitution. Electrochemical measurements and density functional theory calculations indicate that the combination of crystallinity engineering and cobalt substitution in monolayer 2H-MoS2 can not only introduce massive defects that act as new active sites but also activate and make use of the basal plane, which is responsible for the much enhanced HER activity compared to independent crystallinity engineering or cobalt substitution. Impressively, when integrated with a photoharvester cadmium sulfide for photocatalytic hydrogen evolution, the synergistic effect also promotes an excellent cocatalytic performance of monolayer 2H-MoS2 that even higher than platinum (Pt). This study potentially provide new avenues for designing more efficient MoS2-based and other layered materials with enhanced HER performance.