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나노물질 및 화학반응 연구단
나노물질 및 화학반응 연구단
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Intrinsic Relation between Hot Electron Flux and Catalytic Selectivity during Methanol Oxidation

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Title
Intrinsic Relation between Hot Electron Flux and Catalytic Selectivity during Methanol Oxidation
Author(s)
Si Woo Lee; Woonghyeon Park; Hyosun Lee; Hee Chan Song; Yousung Jung; Jeong Young Park
Publication Date
2019-09
Journal
ACS CATALYSIS, v.9, no.9, pp.8424 - 8432
Publisher
AMER CHEMICAL SOC
Abstract
© 2019 American Chemical Society.Catalytic selectivity, or the production of only one desired molecule that may be used as a fuel or chemical out of several thermodynamically possible molecules, is the foundation of surface chemistry. During catalytic reactions, electronic excitation taking place on the surface creates energetic electrons called "hot electrons" that have a significant impact on catalytic reactions. Despite its importance in fundamentally understanding electronic excitation on the surface, no reports show the relation between hot electron flow and catalytic selectivity. Here, using a Pt/n-type TiO2 Schottky nanodiode, we show the intrinsic relation between hot electron flow and catalytic selectivity. On the Pt thin film, hot electron flow was generated by methanol oxidation exhibiting a two-path reaction of either full oxidation to CO2 or partial oxidation to methyl formate; a steady-state chemicurrent was detected. We show that the activation energy of the chemicurrent is quite close to that of the turnover frequency, indicating that the chemicurrent originated from the catalytic reaction on the Pt thin film. The dependence of the chemicurrent on methanol partial pressure was investigated by varying the partial pressure of methanol (1-4 Torr). We show that hot electron generation is more effective in the reaction pathway that produces methyl formate. On the basis of these results, we conclude that the selectivity for methyl formate production correlates well with hot electron generation because of the higher exothermicity of generating the intermediate, as was confirmed using theoretical calculations based on the density functional theory
URI
https://pr.ibs.re.kr/handle/8788114/6267
ISSN
2155-5435
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > Journal Papers (저널논문)
Files in This Item:
ACS Catal. 2019, 9, 8424−8432.pdfDownload

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