Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
School of Materials Science & Engineering, Beihang University, Beijing, 100191, China.
Adv Mater. 2018 Dec;30(51):e1803477. doi: 10.1002/adma.201803477. Epub 2018 Oct 25.
The development of stable and efficient hydrogen evolution reaction (HER) catalysts is essential for the production of hydrogen as a clean energy resource. A combination of experiment and theory demonstrates that the normally inert basal planes of 2D layers of MoS can be made highly catalytically active for the HER when alloyed with rhenium (Re). The presence of Re at the ≈50% level converts the material to a stable distorted tetragonal (DT) structure that shows enhanced HER activity as compared to most of the MoS -based catalysts reported in the literature. More importantly, this new alloy catalyst shows much better stability over time and cycling than lithiated 1T-MoS . Density functional theory calculations find that the role of Re is only to stabilize the DT structure, while catalysis occurs primarily in local Mo-rich DT configurations, where the HER catalytic activity is very close to that in Pt. The study provides a new strategy to improve the overall HER performance of MoS -based materials via chemical doping.
开发稳定、高效的析氢反应（HER）催化剂对于生产清洁的氢能资源至关重要。实验和理论的结合表明，当与铼（Re）合金化时，二维层状 MoS2 的通常惰性基面对于 HER 具有高度的催化活性。当 Re 的含量约为 50%时，材料转化为稳定的扭曲四方（DT）结构，与文献中报道的大多数基于 MoS2 的催化剂相比，表现出增强的 HER 活性。更重要的是，与锂化 1T-MoS2 相比，这种新型合金催化剂在时间和循环过程中表现出更好的稳定性。密度泛函理论计算发现，Re 的作用仅在于稳定 DT 结构，而催化主要发生在局部富 Mo 的 DT 构型中，HER 催化活性非常接近 Pt。该研究为通过化学掺杂提高基于 MoS2 的材料的整体 HER 性能提供了新策略。
