Shedding Light on the Nature of Photoinduced States Formed in a Hydrogen-Generating Supramolecular RuPt Photocatalyst by Ultrafast Spectroscopy

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Abstract

Photoinduced electronic and structural changes of a hydrogen-generating supramolecular RuPt photocatalyst are studied by a combination of time-resolved photoluminescence, optical transient absorption, and X-ray absorption spectroscopy. This work uses the element specificity of X-ray techniques to focus on the interplay between the photophysical and -chemical processes and the associated time scales at the catalytic Pt moiety. We observe very fast (<30 ps) photoreduction of the Pt catalytic site, followed by an ∼600 ps step into a strongly oxidized Pt center. The latter process is likely induced by oxidative addition of reactive iodine species. The oxidized Pt species is long-lived and fully recovers to the original ground state complex on a >10 μs time scale. However, the photosensitizing Ru moiety is fully restored on a much shorter ∼300 ns time scale. This reaction scheme implies that we may withdraw two electrons from a catalyst that is activated by a single photon.

Detaljer

Författare
  • Annemarie Huijser
  • Qing Pan
  • David Van Duinen
  • Mads G. Laursen
  • Amal El Nahhas
  • Pavel Chabera
  • Leon Freitag
  • Leticia González
  • Qingyu Kong
  • Xiaoyi Zhang
  • Kristoffer Haldrup
  • Wesley R. Browne
  • Grigory Smolentsev
  • Jens Uhlig
Enheter & grupper
Externa organisationer
  • University of Twente
  • Technical University of Denmark
  • University of Vienna
  • Argonne National Laboratory
  • University of Groningen
  • Paul Scherrer Institute
  • Southern Federal University
Forskningsområden

Ämnesklassifikation (UKÄ) – OBLIGATORISK

  • Organisk kemi
Originalspråkengelska
Sidor (från-till)6396–6406
TidskriftJournal of Physical Chemistry A
Volym122
Utgåva nummer31
StatusPublished - 2018 jul 27
PublikationskategoriForskning
Peer review utfördJa