Publication:
Operando characterization of an amorphous molybdenum sulfide nanoparticle catalyst during the hydrogen evolution reaction

dc.contributor.coauthorCasalongue, Hernan G. Sanchez
dc.contributor.coauthorBenck, Jesse D.
dc.contributor.coauthorTsai, Charlie
dc.contributor.coauthorKarlsson, Rasmus K. B.
dc.contributor.coauthorNg, May Ling
dc.contributor.coauthorPettersson, Lars G. M.
dc.contributor.coauthorAbild-Pedersen, Frank
dc.contributor.coauthorNorskov, J. K.
dc.contributor.coauthorOgasawara, Hirohito
dc.contributor.coauthorJaramillo, Thomas F.
dc.contributor.coauthorNilsson, Anders
dc.contributor.departmentDepartment of Chemistry
dc.contributor.kuauthorKaya, Sarp
dc.contributor.schoolcollegeinstituteCollege of Sciences
dc.date.accessioned2024-11-09T23:14:25Z
dc.date.issued2014
dc.description.abstractMolybdenum sulfide structures, particularly amorphous MoS3 nanoparticles, are promising materials in the search for cost-effective and scalable water-splitting catalysts. Ex situ observations show that the nanoparticles exhibit a composition change from MoS3 to defective MoS2 when subjected to hydrogen evolution reaction (HER) conditions, raising questions regarding the active surface sites taking part in the reaction. We tracked the in situ transformation of amorphous MoS3 nanoparticles under HER conditions through ambient pressure X-ray photoelectron spectroscopy and performed density functional theory studies of model MoSx systems. We demonstrate that, under operating conditions, surface sites are converted from MoS3 to MoS2 in a gradual manner and that the electrolytic current densities are proportional to the extent of the transformation. We also posit that it is the MoS2 edge-like sites that are active during HER, with the high activity of the catalyst being attributed to the increase in surface MoS2 edge-like sites after the reduction of MoS3 sites.
dc.description.indexedbyWOS
dc.description.indexedbyScopus
dc.description.issue50
dc.description.openaccessNO
dc.description.publisherscopeInternational
dc.description.sponsoredbyTubitakEuN/A
dc.description.sponsorshipJoint Center for Artificial Photosynthesis [DE-SC0004993]
dc.description.sponsorshipPrecursory Research for Embryonic Science and Technology (PRESTO), Japan Science and Technology Agency (JST)
dc.description.sponsorshipCenter on Nanostructuring for Efficient Energy Conversion (CNEEC) at Stanford University, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001060]
dc.description.sponsorshipU.S. Department of Energy (DOE), Office of Basic Energy Sciences
dc.description.sponsorshipNational Science Foundation [DGE-114747]
dc.description.sponsorshipSwedish Energy Agency
dc.description.sponsorshipPermascand AB This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: the experimental work was supported by the Joint Center for Artificial Photosynthesis Award DE-SC0004993. H.O. gratefully acknowledges the support from Precursory Research for Embryonic Science and Technology (PRESTO), Japan Science and Technology Agency (JST). Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource (SSRL), a division of SLAC National Accelerator Laboratory and an Office of Science user facility operated by Stanford University for the U.S. Department of Energy. For work on molybdenum sulfide catalyst synthesis and development (J.D.B. and T.F.J.) and the DFT free-energy calculations (C.T, F.A-P., J.K.N), we acknowledge support by the Center on Nanostructuring for Efficient Energy Conversion (CNEEC) at Stanford University, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DE-SC0001060. C.T, M.L.N., F.A-P., J.K.N., and A.N. acknowledge financial support from the U.S. Department of Energy (DOE), Office of Basic Energy Sciences to the SUNCAT Center for Interface Science and Catalysis. C.T. acknowledges support from the National Science Foundation Graduate Research Fellowship Program (GRFP) Grant DGE-114747. R.K.B.K. acknowledges financial support from the Swedish Energy Agency and Permascand AB. XPS chemical shift calculations were performed using the resources of the High Performance Computing Center North (HPC2N), as provided by the Swedish National Infrastructure for Computing (SNIC).
dc.description.volume118
dc.identifier.doi10.1021/jp505394e
dc.identifier.eissn1932-7455
dc.identifier.issn1932-7447
dc.identifier.quartileQ2
dc.identifier.scopus2-s2.0-84949116763
dc.identifier.urihttps://doi.org/10.1021/jp505394e
dc.identifier.urihttps://hdl.handle.net/20.500.14288/10155
dc.identifier.wos346759300037
dc.keywordsActive edge sites
dc.keywordsIn-situ
dc.keywordsAb-initio
dc.keywordsMos2
dc.language.isoeng
dc.publisherAmerican Chemical Society (ACS)
dc.relation.ispartofJournal of Physical Chemistry C
dc.subjectChemistry
dc.subjectPhysical chemistry
dc.subjectNanoscience
dc.subjectNanotechnology
dc.subjectMaterials science
dc.titleOperando characterization of an amorphous molybdenum sulfide nanoparticle catalyst during the hydrogen evolution reaction
dc.typeJournal Article
dspace.entity.typePublication
local.contributor.kuauthorKaya, Sarp
local.publication.orgunit1College of Sciences
local.publication.orgunit2Department of Chemistry
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relation.isOrgUnitOfPublication.latestForDiscovery035d8150-86c9-4107-af16-a6f0a4d538eb
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