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Active repair of a dinuclear photocatalyst for visible-light-driven hydrogen production.
Pfeffer, Michael G; Müller, Carolin; Kastl, Evelyn T E; Mengele, Alexander K; Bagemihl, Benedikt; Fauth, Sven S; Habermehl, Johannes; Petermann, Lydia; Wächtler, Maria; Schulz, Martin; Chartrand, Daniel; Laverdière, François; Seeber, Phillip; Kupfer, Stephan; Gräfe, Stefanie; Hanan, Garry S; Vos, Johannes G; Dietzek-Ivansic, Benjamin; Rau, Sven.
Afiliación
  • Pfeffer MG; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Müller C; Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, Germany.
  • Kastl ETE; Leibniz Institute of Photonic Technology, Jena, Germany.
  • Mengele AK; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Bagemihl B; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Fauth SS; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Habermehl J; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Petermann L; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Wächtler M; Institute of Inorganic Chemistry I (Materials and Catalysis), Ulm University, Ulm, Germany.
  • Schulz M; Leibniz Institute of Photonic Technology, Jena, Germany.
  • Chartrand D; Abbe Center of Photonics, Jena, Germany.
  • Laverdière F; Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, Germany.
  • Seeber P; Department of Chemistry, University of Montréal, Montréal, Québec, Canada.
  • Kupfer S; Department of Chemistry, University of Montréal, Montréal, Québec, Canada.
  • Gräfe S; Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, Germany.
  • Hanan GS; Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, Germany.
  • Vos JG; Institute of Physical Chemistry, Friedrich Schiller University Jena, Jena, Germany.
  • Dietzek-Ivansic B; Department of Chemistry, University of Montréal, Montréal, Québec, Canada.
  • Rau S; SRC for Solar Energy Conversion, School of Chemical Sciences, Dublin City University, Dublin, Ireland.
Nat Chem ; 14(5): 500-506, 2022 05.
Article en En | MEDLINE | ID: mdl-35132222
The molecular apparatus behind biological photosynthesis retains its long-term functionality through enzymatic repair. However, bioinspired molecular devices designed for artificial photosynthesis, consisting of a photocentre, a bridging ligand and a catalytic centre, can become unstable and break down when their individual modules are structurally compromised, halting their overall functionality and operation. Here we report the active repair of such an artificial photosynthetic molecular device, leading to complete recovery of catalytic activity. We have identified the hydrogenation of the bridging ligand, which inhibits the light-driven electron transfer between the photocentre and catalytic centre, as the deactivation mechanism. As a means of repair, we used the light-driven generation of singlet oxygen, catalysed by the photocentre, to enable the oxidative dehydrogenation of the bridging unit, which leads to the restoration of photocatalytic hydrogen formation.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Fotosíntesis / Luz Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Reino Unido
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Fotosíntesis / Luz Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Reino Unido