Molecular Porous Photosystems Tailored for Long-Term Photocatalytic CO2 Reduction

RMN+ECI2D:ING+FWI:AGH:YMO:CLO:DFA:JECInternational audienceHerein, we report the molecular-level structuration of two full photosystems into conjugated porous organic polymers. The strategy of heterogenization gives rise to photosystems which are still fully active after 4 days of continuous illumination. Those materials catalyse 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 singleframework 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