Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide

Stanley S. Chou (), Na Sai, Ping Lu, Eric N. Coker, Sheng Liu, Kateryna Artyushkova, Ting S. Luk, Bryan Kaehr and C. Jeffrey Brinker ()
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Stanley S. Chou: Advanced Materials Laboratory, Sandia National Laboratories
Na Sai: The University of Texas at Austin
Ping Lu: Sandia National Laboratories
Eric N. Coker: Advanced Materials Laboratory, Sandia National Laboratories
Sheng Liu: Center For Integrated Nanotechnologies (CINT), Sandia National Laboratories
Kateryna Artyushkova: The University of New Mexico
Ting S. Luk: Center For Integrated Nanotechnologies (CINT), Sandia National Laboratories
Bryan Kaehr: Advanced Materials Laboratory, Sandia National Laboratories
C. Jeffrey Brinker: Advanced Materials Laboratory, Sandia National Laboratories

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract Establishing processing–structure–property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔGH), and, with respect to catalysis, the 1T′ transformation renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Indeed, we show basal plane activation of 1T′ molybdenum disulfide and a lowering of ΔGH from +1.6 eV for 2H to +0.18 eV for 1T′, comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.

Date: 2015
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DOI: 10.1038/ncomms9311

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