Molecular Porous Photosystems Tailored for Long-Term Photocatalytic CO
CO2 reduction
density functional calculations
in situ time-resolved spectroscopy
photocatalysis
porous polymers
Journal
Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543
Informations de publication
Date de publication:
23 Mar 2020
23 Mar 2020
Historique:
received:
09
10
2019
revised:
06
01
2020
pubmed:
17
1
2020
medline:
17
1
2020
entrez:
17
1
2020
Statut:
ppublish
Résumé
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.
Identifiants
pubmed: 31945254
doi: 10.1002/anie.201912883
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
5116-5122Subventions
Organisme : Deutsche Forschungsgemeinschaft
ID : WI 4721/1-1
Organisme : Deutsche Forschungsgemeinschaft
ID : EXC 2186
Organisme : Erasmus+
ID : FPA 2013-0037
Organisme : Chevreul institute
ID : FR 2638
Organisme : CNRS
ID : Momentum 2018 excellence grant
Informations de copyright
© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
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