Single-Site Photocatalytic H2 Evolution from Covalent Organic Frameworks with 
Molecular Cobaloxime Co-Catalysts

Banerjee, T.; Haase, F.; Savasci, G.; Gottschling, K.; Ochsenfeld, C.; Lotsch, B. V.

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Single-Site Photocatalytic H₂ Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts

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Haase, F.
Department Nanochemistry (Bettina V. Lotsch), Max Planck Institute for Solid State Research, Max Planck Society;

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Lotsch, B. V.
Department Nanochemistry (Bettina V. Lotsch), Max Planck Institute for Solid State Research, Max Planck Society;

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Citation

Banerjee, T., Haase, F., Savasci, G., Gottschling, K., Ochsenfeld, C., & Lotsch, B. V. (2017). Single-Site Photocatalytic H₂ Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts. Journal of the American Chemical Society, 139(45), 16228-16234.

Cite as: https://hdl.handle.net/21.11116/0000-000E-D156-5

Abstract

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.