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Characterization of the Platinum–Hydrogen Bond by Surface-Sensitive Time-Resolved Infrared Spectroscopy


Paleček, David; Tek, Gökçen; Lan, Jinggang; Iannuzzi, Marcella; Hamm, Peter (2018). Characterization of the Platinum–Hydrogen Bond by Surface-Sensitive Time-Resolved Infrared Spectroscopy. Journal of Physical Chemistry Letters, (9):1254-1259.

Abstract

The vibrational dynamics of Pt-H on a nanostructured platinum surface has been examined by ultrafast infrared spectroscopy. Three bands are observed at 1800, 2000, and 2090 cm-1, which are assigned to Pt-CO in a bridged and linear configuration and Pt-H, respectively. Lifetime analysis revealed a time constant of (0.8 ± 0.1) ps for the Pt-H mode, considerably shorter than that of Pt-CO because of its stronger coupling to the metal substrate. Two-dimensional attenuated total reflection infrared spectroscopy provided additional evidence for the assignment based on the anharmonic shift, which is large in the case of Pt-H (90 cm-1), in agreement with the density functional theory calculations. The absorption cross section of Pt-H is smaller than that of the very strong Pt-CO vibration by only a modest factor of ∼1.5-3. Because Pt-H is transiently involved in catalytic water splitting on Pt, the present spectroscopic characterization paves the way for in-operando kinetic studies of such reactions.

Abstract

The vibrational dynamics of Pt-H on a nanostructured platinum surface has been examined by ultrafast infrared spectroscopy. Three bands are observed at 1800, 2000, and 2090 cm-1, which are assigned to Pt-CO in a bridged and linear configuration and Pt-H, respectively. Lifetime analysis revealed a time constant of (0.8 ± 0.1) ps for the Pt-H mode, considerably shorter than that of Pt-CO because of its stronger coupling to the metal substrate. Two-dimensional attenuated total reflection infrared spectroscopy provided additional evidence for the assignment based on the anharmonic shift, which is large in the case of Pt-H (90 cm-1), in agreement with the density functional theory calculations. The absorption cross section of Pt-H is smaller than that of the very strong Pt-CO vibration by only a modest factor of ∼1.5-3. Because Pt-H is transiently involved in catalytic water splitting on Pt, the present spectroscopic characterization paves the way for in-operando kinetic studies of such reactions.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:23 February 2018
Deposited On:09 Mar 2018 14:36
Last Modified:18 Apr 2018 11:49
Publisher:American Chemical Society (ACS)
ISSN:1948-7185
Funders:Swiss National Science Foundation, University Research Priority Program LightChEC (URPP)
Additional Information:This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Cehmistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpclett.8b00310.
OA Status:Closed
Publisher DOI:https://doi.org/10.1021/acs.jpclett.8b00310
Project Information:
  • : FunderSNSF
  • : Grant ID
  • : Project TitleSwiss National Science Foundation
  • : Funder
  • : Grant ID
  • : Project TitleUniversity Research Priority Program LightChEC (URPP)

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Embargo till: 2019-02-23