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Banerjee, Tanmay; Haase, Frederik; Savasci, Goekcen; Gottschling, Kerstin; Ochsenfeld, Christian; Lotsch, Bettina V. (2017): Single-Site Photocatalytic H-2 Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts. In: Journal of the American Chemical Society, Vol. 139, No. 45: pp. 16228-16234
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We demonstrate photocatalytic hydrogen evolution using COF photosensitizers with molecular proton reduction catalysts for the first time. With azine-linked N2-COF photosensitizer, chloro(pyridine)cobaloxime co-catalyst, and TEOA donor, H-2 evolution rate of 782,mu mol h(-1) g(-1) and TON of 54.4 has been obtained in a water/acetonitrile mixture. PXRD, solid-state spectroscopy, EM analysis, and quantum-chemical calculations suggest an outer sphere electron transfer from the COF to the co-catalyst which subsequently follows a monometallic pathway of H-2 generation from the Co-III-hydride and/or Co-II-hydride species.