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

Lefebvre, Jean-Francois; Schindler, Julian; Traber, Philipp; Zhang, Ying; Kupfer, Stephan; Gräfe, Stefanie; Baussanne, Isabelle; Demeunynck, Martine; Mouesca, Jean-Marie; Gambarelli, Serge; Artero, Vincent; Dietzek, Benjamin; Chavarot-Kerlidou, Murielle
in: Chemical Science (2018) 4152

Increasing the efficiency of molecular artificial photosynthetic systems is mandatory for the construction of functional devices for solar fuels 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 DFT studies allowed to localize the two electron-storage sites and to relate charge photoaccumulation with proton-coupled electron transfer processes.

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