Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts

[Image: see text] 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 μmol h(–1) g(–1) an...

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Autores principales: Banerjee, Tanmay, Haase, Frederik, Savasci, Gökcen, Gottschling, Kerstin, Ochsenfeld, Christian, Lotsch, Bettina V.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5691321/
https://www.ncbi.nlm.nih.gov/pubmed/29022345
http://dx.doi.org/10.1021/jacs.7b07489
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author Banerjee, Tanmay
Haase, Frederik
Savasci, Gökcen
Gottschling, Kerstin
Ochsenfeld, Christian
Lotsch, Bettina V.
author_facet Banerjee, Tanmay
Haase, Frederik
Savasci, Gökcen
Gottschling, Kerstin
Ochsenfeld, Christian
Lotsch, Bettina V.
author_sort Banerjee, Tanmay
collection PubMed
description [Image: see text] 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 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 H(2) generation from the Co(III)-hydride and/or Co(II)-hydride species.
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spelling pubmed-56913212017-11-18 Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts Banerjee, Tanmay Haase, Frederik Savasci, Gökcen Gottschling, Kerstin Ochsenfeld, Christian Lotsch, Bettina V. J Am Chem Soc [Image: see text] 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 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 H(2) generation from the Co(III)-hydride and/or Co(II)-hydride species. American Chemical Society 2017-10-12 2017-11-15 /pmc/articles/PMC5691321/ /pubmed/29022345 http://dx.doi.org/10.1021/jacs.7b07489 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Attribution (CC-BY) License (http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html) , which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
spellingShingle Banerjee, Tanmay
Haase, Frederik
Savasci, Gökcen
Gottschling, Kerstin
Ochsenfeld, Christian
Lotsch, Bettina V.
Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title_full Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title_fullStr Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title_full_unstemmed Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title_short Single-Site Photocatalytic H(2) Evolution from Covalent Organic Frameworks with Molecular Cobaloxime Co-Catalysts
title_sort single-site photocatalytic h(2) evolution from covalent organic frameworks with molecular cobaloxime co-catalysts
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5691321/
https://www.ncbi.nlm.nih.gov/pubmed/29022345
http://dx.doi.org/10.1021/jacs.7b07489
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