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Journal Article
Research Support, Non-U.S. Gov't
Single-Site Photocatalytic H 2 Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts.
Journal of the American Chemical Society 2017 November 16
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, H2 evolution rate of 782 μmol 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 H2 generation from the CoIII -hydride and/or CoII -hydride species.
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