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Molecular Porous Photosystems Tailored for Long‐Term Photocatalytic CO 2 Reduction
Author(s) -
Wisser Florian M.,
Duguet Mathis,
Perrinet Quentin,
Ghosh Ashta C.,
AlvesFavaro Marcelo,
Mohr Yorck,
Lorentz Chantal,
Quadrelli Elsje Alessandra,
Palkovits Regina,
Farrusseng David,
MellotDraznieks Caroline,
Waele Vincent,
Canivet Jérôme
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201912883
Subject(s) - photochemistry , photosystem , catalysis , formate , chemistry , photocatalysis , electron transfer , moiety , visible spectrum , conjugated system , chromophore , photoredox catalysis , covalent bond , materials science , polymer , photosystem ii , organic chemistry , optoelectronics , photosynthesis , biochemistry
The molecular‐level structuration of two full photosystems into conjugated porous organic polymers is reported. The strategy of heterogenization gives rise to photosystems which are still fully active after 4 days of continuous illumination. Those materials catalyze the carbon dioxide photoreduction driven by visible light to produce up to three grams of formate per gram of catalyst. The covalent tethering of the two active sites into a single framework is shown to play a key role in the visible light activation of the catalyst. The unprecedented long‐term efficiency arises from an optimal photoinduced electron transfer from the light harvesting moiety to the catalytic site as anticipated by quantum mechanical calculations and evidenced by in situ ultrafast time‐resolved spectroscopy.