期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 13, 页码 5116-5122出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201912883
关键词
CO2 reduction; density functional calculations; in situ time-resolved spectroscopy; photocatalysis; porous polymers
资金
- Deutsche Forschungsgemeinschaft (DFG) [WI 4721/1-1]
- CNRS through Momentum 2018 excellence grant
- SINCHEM Joint Doctorate programme under the Erasmus Mundus Action 1 Programme [FPA 2013-0037]
- German Excellence Initiative [EXC 2186]
- Chevreul institute [FR 2638]
- Ministre de lEnseignement Suprieur et de la Recherche
- Rgion Nord-Pas de Calais
- FEDER
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.
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