Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/ncomms9311
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Science Program [DE-FG02-02ER15368]
- Sandia National Laboratories
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- U.S. Department of Energy (DOE) [DE-FG02-02ER15368] Funding Source: U.S. Department of Energy (DOE)
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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 (Delta G(H)), 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 Delta G(H) 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.
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