Engineering MoS2 Basal Planes for Hydrogen Evolution via Synergistic Ruthenium Doping and Nanocarbon Hybridization
Engineering MoS2 Basal Planes for Hydrogen Evolution via Synergistic Ruthenium Doping and Nanocarbon Hybridization
复制标题
DOI：
10.1002/advs.201900090
复制
发表时间：
2019-03
期刊：
影响因子：
15.1
通讯作者：
Xing Zhang;F. Zhou;S. Zhang;Yongye Liang;Ruihu Wang
中科院分区：
文献类型：
--
作者：
Xing Zhang;F. Zhou;S. Zhang;Yongye Liang;Ruihu Wang
提高二维层状金属二硫化物基面位的固有活性和可及性是优化其能量转化和储存的催化性能所必需的。本文报道了一种核/壳结构的杂化催化剂，其特征是钌（Ru）掺杂二硫化钼（MoS2）纳米片紧密包裹在多壁碳纳米管（CNT）周围，用于高效析氢反应（HER）。当5 at%（原子百分数）Ru取代MoS2中的Mo时，Ru‐MoS2/CNT获得了最佳的HER活性，在−10 mA cm−2下显示出50 mV的小过电位，在1 m KOH下显示出62 mV dec−1的低Tafel斜率。理论模拟表明，钌与6个S原子配位取代Mo是热力学稳定的，与钌掺杂剂相邻的平面内S原子代表了促进水吸附、解离和氢吸附/解吸的新活性中心。这项工作为协同提高过渡金属二硫族化合物的HER活性提供了一种多尺度结构和电子工程策略。
Promoting the intrinsic activity and accessibility of basal plane sites in 2D layered metal dichalcogenides is desirable to optimize their catalytic performance for energy conversion and storage. Herein, a core/shell structured hybrid catalyst, which features few‐layered ruthenium (Ru)‐doped molybdenum disulfide (MoS2) nanosheets closely sheathing around multiwalled carbon nanotube (CNT), for highly efficient hydrogen evolution reaction (HER) is reported. With 5 at% (atomic percent) Ru substituting for Mo in MoS2, Ru‐MoS2/CNT achieves the optimum HER activity, which displays a small overpotential of 50 mV at −10 mA cm−2 and a low Tafel slope of 62 mV dec−1 in 1 m KOH. Theoretical simulations reveal that Ru substituting for Mo in coordination with six S atoms is thermodynamically stable, and the in‐plane S atoms neighboring Ru dopants represent new active centers for facilitating water adsorption, dissociation, and hydrogen adsorption/desorption. This work provides a multiscale structural and electronic engineering strategy for synergistically enhancing the HER activity of transition metal dichalcogenides.