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Shedding Light on the Nature of Photoinduced States Formed in a Hydrogen-Generating Supramolecular RuPt Photocatalyst by Ultrafast Spectroscopy.
Huijser, Annemarie; Pan, Qing; van Duinen, David; Laursen, Mads G; El Nahhas, Amal; Chabera, Pavel; Freitag, Leon; González, Leticia; Kong, Qingyu; Zhang, Xiaoyi; Haldrup, Kristoffer; Browne, Wesley R; Smolentsev, Grigory; Uhlig, Jens.
Afiliación
  • Huijser A; Optical Sciences and PhotoCatalytic Synthesis Groups, MESA+ Institute , University of Twente , P.O. Box 217, 7500 AE Enschede , The Netherlands.
  • Pan Q; Optical Sciences and PhotoCatalytic Synthesis Groups, MESA+ Institute , University of Twente , P.O. Box 217, 7500 AE Enschede , The Netherlands.
  • van Duinen D; Optical Sciences and PhotoCatalytic Synthesis Groups, MESA+ Institute , University of Twente , P.O. Box 217, 7500 AE Enschede , The Netherlands.
  • Laursen MG; Department of Physics , Technical University of Denmark , 2800 Kongens Lyngby , Denmark.
  • El Nahhas A; Department of Chemical Physics , Lund University , Getingevägen 60 , Lund 22100 , Sweden.
  • Chabera P; Department of Chemical Physics , Lund University , Getingevägen 60 , Lund 22100 , Sweden.
  • Freitag L; Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , 1090 Vienna , Austria.
  • González L; Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , 1090 Vienna , Austria.
  • Kong Q; X-ray Sciences Division , Argonne National Laboratory , Argonne , Illinois 60439 , United States.
  • Zhang X; X-ray Sciences Division , Argonne National Laboratory , Argonne , Illinois 60439 , United States.
  • Haldrup K; Department of Physics , Technical University of Denmark , 2800 Kongens Lyngby , Denmark.
  • Browne WR; Molecular Inorganic Chemistry Group, Stratingh Institute for Chemistry , University of Groningen , 9747 AG Groningen , The Netherlands.
  • Smolentsev G; Paul Scherrer Institute , Villigen 5232 , Switzerland.
  • Uhlig J; Smart Materials International Research Center , Southern Federal University of Russia , Rostov-on-Don 344090 , Russian Federation.
J Phys Chem A ; 122(31): 6396-6406, 2018 Aug 09.
Article en En | MEDLINE | ID: mdl-30052048
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.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2018 Tipo del documento: Article País de afiliación: Países Bajos Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem A Asunto de la revista: QUIMICA Año: 2018 Tipo del documento: Article País de afiliación: Países Bajos Pais de publicación: Estados Unidos