An artificial photosynthetic system for photoaccumulation of two electrons on a fused dipyridophenazine (dppz)-pyridoquinolinone ligand

Chemical Science
Jean-François LefebvreMurielle Chavarot-Kerlidou

Abstract

Increasing the efficiency of molecular artificial photosynthetic systems is mandatory for the construction of functional devices for solar fuel production. Decoupling the light-induced charge separation steps from the catalytic process is a promising strategy, which can be achieved thanks to the introduction of suitable electron relay units performing charge accumulation. We report here on a novel ruthenium tris-diimine complex able to temporarily store two electrons on a fused dipyridophenazine-pyridoquinolinone π-extended ligand upon visible-light irradiation in the presence of a sacrificial electron donor. Full characterization of this compound and of its singly and doubly reduced derivatives thanks to resonance Raman, EPR and (TD)DFT studies allowed us to localize the two electron-storage sites and to relate charge photoaccumulation with proton-coupled electron transfer processes.

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Citations

Aug 10, 2018·Chemistry : a European Journal·Julia NomrowskiOliver S Wenger
Aug 29, 2018·Chemistry : a European Journal·Keiya YamamotoKen Sakai
Feb 28, 2019·Chemical Communications : Chem Comm·Andrea Pannwitz, Oliver S Wenger
Apr 30, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Rajaa FarranJérôme Chauvin
Jul 25, 2019·Chemistry : a European Journal·Nicholas M RandellMurielle Chavarot-Kerlidou
Jan 17, 2020·Angewandte Chemie·Felix GlaserOliver S Wenger
Dec 10, 2020·Chemical Society Reviews·Christine Kranz, Maria Wächtler
Jul 20, 2018·The Journal of Physical Chemistry. a·Julian SchindlerBenjamin Dietzek
Apr 14, 2018·Journal of the American Chemical Society·Julia Nomrowski, Oliver S Wenger
Jun 27, 2019·ACS Applied Materials & Interfaces·Xiao-Xin LiYa-Qian Lan
Aug 25, 2020·Journal of the American Chemical Society·Martin SchulzBenjamin Dietzek
Dec 4, 2021·Physical Chemistry Chemical Physics : PCCP·Carolin MüllerBenjamin Dietzek-Ivanšić

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Methods Mentioned

BETA
electronic paramagnetic resonance

Software Mentioned

TDDFT

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