Activating Catalytic Inert Basal Plane of Molybdenum Disulfide to Optimize Hydrogen Evolution Activity via Defect Doping and Strain Engineering

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• 作者：Guoping Gao ; Qiao Sun ; Aijun Du
• 刊名：Journal of Physical Chemistry C
• 出版年：2016
• 出版时间：August 4, 2016
• 年：2016
• 卷：120
• 期：30
• 页码：16761-16766
• 全文大小：353K
• 年卷期：0
• ISSN：1932-7455

文摘

Molybdenum disulfide (MoS₂) is a promising alternative hydrogen evolution reaction (HER) catalyst to high-cost platinum (Pt) due to its large surface area, low cost, easy preparation, and earth abundance. The HER efficiency of MoS₂ remains low because only the edge S-sites are active for the HER. In this work, two practical strategies, heteroatom doping (Rh, Pd, and Ag) and strain engineering, are proposed to activate the inert in-plane S-site for the HER. The density functional theory calculations demonstrate that doping MoS₂ with heteroatom can trigger the HER activity of the S atoms next to the doping atoms, with a negative hydrogen adsorption free energy (ΔG_H*⁰). The negative ΔG_H*⁰ can be further significantly optimized by a small compressive strain. Therefore, the combination of heteroatom doping and a small compressive strain can yield an ideal value of hydrogen-binding free energy (ΔG_H*⁰ = 0 eV) for HER. These results highlight an innovative avenue to optimize the HER performance of MoS₂.