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Petermann L, Staehle R, Pfeifer M, et al. Oxygen-Dependent Photocatalytic Water Reduction with a Ruthenium(imidazolium) Chromophore and a Cobaloxime Catalyst. Chemistry. 2016;22(24):8240-53doi: 10.1002/chem.201505113.
Petermann, L., Staehle, R., Pfeifer, M., Reichardt, C., Sorsche, D., Wächtler, M., Popp, J., Dietzek, B., & Rau, S. (2016). Oxygen-Dependent Photocatalytic Water Reduction with a Ruthenium(imidazolium) Chromophore and a Cobaloxime Catalyst. Chemistry (Weinheim an der Bergstrasse, Germany), 22(24), 8240-53. https://doi.org/10.1002/chem.201505113
Petermann, Lydia, et al. "Oxygen-Dependent Photocatalytic Water Reduction with a Ruthenium(imidazolium) Chromophore and a Cobaloxime Catalyst." Chemistry (Weinheim an der Bergstrasse, Germany) vol. 22,24 (2016): 8240-53. doi: https://doi.org/10.1002/chem.201505113
Petermann L, Staehle R, Pfeifer M, Reichardt C, Sorsche D, Wächtler M, Popp J, Dietzek B, Rau S. Oxygen-Dependent Photocatalytic Water Reduction with a Ruthenium(imidazolium) Chromophore and a Cobaloxime Catalyst. Chemistry. 2016 Jun 06;22(24):8240-53. doi: 10.1002/chem.201505113. Epub 2016 May 02. PMID: 27135804.
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Chemistry. 2016 Jun 06;22(24):8240-53. doi: 10.1002/chem.201505113. Epub 2016 May 02.

Oxygen-Dependent Photocatalytic Water Reduction with a Ruthenium(imidazolium) Chromophore and a Cobaloxime Catalyst.

Chemistry (Weinheim an der Bergstrasse, Germany)

Lydia Petermann, Robert Staehle, Maxim Pfeifer, Christian Reichardt, Dieter Sorsche, Maria Wächtler, Jürgen Popp, Benjamin Dietzek, Sven Rau

Affiliations

  1. Institute of Inorganic Chemistry, Materials and Catalysis, University of Ulm, Albert-Einstein-Allee 11, 89081, Ulm, Germany), Fax.
  2. Solid State Chemistry, Helmholtz Institute Ulm (HIU), Helmholtzstraße 11, 89081, Ulm, Germany.
  3. Institute of Physical Chemistry and Abbe Center of Photonics, Friedrich Schiller University Jena, Helmholtzweg 4, 07743, Jena, Germany.
  4. Leibniz Institute of Photonic Technology (IPHT), Albert-Einstein-Straße 9, 07745, Jena, Germany.
  5. Jena Center for Soft Matter (JCSM), Friedrich Schiller University Jena, Philosophenweg 7, 07743, Jena, Germany.
  6. Institute of Inorganic Chemistry, Materials and Catalysis, University of Ulm, Albert-Einstein-Allee 11, 89081, Ulm, Germany), Fax. [email protected].

PMID: 27135804 DOI: 10.1002/chem.201505113

Abstract

Detailed investigations of a photocatalytic system capable of producing hydrogen under pre-catalytic aerobic conditions are reported. This system consists of the NHC precursor chromophore [Ru(tbbpy)2 (RR'ip)][PF6 ]3 (abbreviated as Ru(RR'ip)[PF6 ]3 ; tbbpy=4,4'-di-tert-butyl-2,2'-bipyridine, RR'ip=1,3-disubstituted-1H-imidazo[4,5-f][1,10]phenanthrolinium), the reduction catalyst Co(dmgH)2 (dmgH=dimethylglyoximato), and the electron donor ascorbic acid (AA). Screening studies with respect to solvent, cobaloxime catalyst, electron donor, pH, and concentrations of the individual components yielded optimized photocatalytic conditions. The system shows high activity based on Ru, with turnover numbers up to 2000 under oxygen-free and pre-catalytic aerobic conditions. The turnover frequency in the latter case was even higher than that for the oxygen-free catalyst system. The Ru complexes show high photostability and their first excited state is primarily located on the RR'ip ligand. X-ray crystallographic analysis of the rigid cyclophane-type ligand dd(ip)2 (Br)2 (dd(ip)2 =1,1',3,3'-bis(2,3,5,6-tetramethyl-1,4-phenylene)bis(methylene)bis(1H-imidazo[4,5-f][1,10]phenanthrolinium)) and the catalytic activity of its Ru complex [{(tbbpy)2 Ru}2 (μ-dd(ip)2 )][PF6 ]6 (abbreviated as Ru2 (dd(ip)2 )[PF6 ]6 ) suggest an intermolecular catalytic cycle.

© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords: N-heterocyclic carbene precursors; hydrogen; photocatalysis; pre-catalytic aerobic conditions; ruthenium

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