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- W3048253835 abstract "Unlike metal or semiconductorelectrodes, the surface charge resultingfrom the protonation or deprotonation of insulating mineral oxidesis highly localized and heterogeneous in nature. In this work theStark active CN stretch of potassium thiocyanate is used asa molecular probe of the heterogeneity of the interfacial electrostaticpotential at the α-Al2O3(0001)/H2O interface. Vibrational sum frequency generation (vSFG) measurementsperformed in the OH stretching region suggest that thiocyanate speciesorganize interfacial water similarly to halide ions. Changes in theelectrostatic potential are then tracked via Stark shifts of the vibrationalfrequency of the thiocyanate stretch. Our vSFG measurements show thatwe can simultaneously measure the vSFG response of SCN– ions experiencing charged and neutral surface sites. We assign localpotentials of +308 and −154 mV to positively and negativelycharged aluminol groups that are present at pH = 4 and pH = 10, respectively.Thiocyanate anions at positively charged surface sites and negativelycharged surface sites and those participating in contact ion pairingadopt similar orientations and are oppositely oriented relative tothiocyanate ions near neutral surface sites. All four species followedLangmuir adsorption isotherms. Density functional theory–moleculardynamics (DFT-MD) simulations of SCN– near the neutralα-Al2O3(0001)/H2O interfaceshow that the vSFG response in the CN stretch region originatesfrom a SCN–H–O–Al complex, suggesting the surfacesite specificity of these experiments. To our knowledge this is thefirst spectroscopic measurement of local potentials associated witha heterogeneously charged surface. The ability to probe the evolutionof local charges in situ could provide vital insight into many industrial,electrochemical, and geochemically relevant interfaces." @default.
- W3048253835 created "2020-08-13" @default.
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- W3048253835 date "2020-07-06" @default.
- W3048253835 modified "2023-09-24" @default.
- W3048253835 title "ProbingHeterogeneous Charge Distributions at theα‑Al2O3(0001)/H2O Interface" @default.
- W3048253835 doi "https://doi.org/10.1021/jacs.0c01366.s001" @default.
- W3048253835 hasPublicationYear "2020" @default.
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