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dc.contributor.authorWesley, Thejas S
dc.contributor.authorHülsey, Max J
dc.contributor.authorWestendorff, Karl S
dc.contributor.authorLewis, Noah B
dc.contributor.authorCrumlin, Ethan J
dc.contributor.authorRomán-Leshkov, Yuriy
dc.contributor.authorSurendranath, Yogesh
dc.date.accessioned2024-09-20T18:13:11Z
dc.date.available2024-09-20T18:13:11Z
dc.date.issued2023
dc.identifier.urihttps://hdl.handle.net/1721.1/156921
dc.description.abstractElectrochemical polarization, which often plays a critical role in driving chemical reactions at solid–liquid interfaces, can arise spontaneously through the exchange of ions and/or electrons across the interface. However, the extent to which such spontaneous polarization prevails at nonconductive interfaces remains unclear because such materials preclude measuring and controlling the degree of interfacial polarization via standard (i.e., wired) potentiometric methods. Herein, we circumvent the limitations of wired potentiometry by applying infrared and ambient pressure X-ray photoelectron spectroscopies (AP-XPS) to probe the electrochemical potential of nonconductive interfaces as a function of solution composition. As a model class of macroscopically nonconductive interfaces, we specifically probe the degree of spontaneous polarization of ZrO2-supported Pt and Au nanoparticles immersed in aqueous solutions of varying pH. Shifts in the Pt-adsorbed CO vibrational band position evince electrochemical polarization of the Pt/ZrO2–water interface with changing pH, and AP-XPS reveals quasi-Nernstian shifts of the electrochemical potential of Pt and Au with pH in the presence of H2. These results indicate that spontaneous proton transfer via equilibrated H+/H2 interconversion spontaneously polarizes metal nanoparticles even when supported on a nonconductive host. Consequently, these findings indicate that solution composition (i.e., pH) can be an effective handle for tuning interfacial electrical polarization and potential at nonconductive interfaces.en_US
dc.language.isoen
dc.publisherRoyal Society of Chemistryen_US
dc.relation.isversionof10.1039/d3sc00884cen_US
dc.rightsCreative Commons Attribution-Noncommercialen_US
dc.rights.urihttp://creativecommons.org/licenses/by-nc/3.0/en_US
dc.sourceRoyal Society of Chemistryen_US
dc.titleMetal nanoparticles supported on a nonconductive oxide undergo pH-dependent spontaneous polarizationen_US
dc.typeArticleen_US
dc.identifier.citationChem. Sci., 2023,14, 7154-7160en_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Chemical Engineeringen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Chemistryen_US
dc.relation.journalChemical Scienceen_US
dc.eprint.versionFinal published versionen_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dc.date.updated2024-09-20T18:03:41Z
dspace.orderedauthorsWesley, TS; Hülsey, MJ; Westendorff, KS; Lewis, NB; Crumlin, EJ; Román-Leshkov, Y; Surendranath, Yen_US
dspace.date.submission2024-09-20T18:03:43Z
mit.journal.volume14en_US
mit.journal.issue26en_US
mit.licensePUBLISHER_CC
mit.metadata.statusAuthority Work and Publication Information Neededen_US


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