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Synthesis and hydrogen evolving catalysis of a panchromatic photochemical molecular device

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Abstract

A dinuclear hydrogen evolution photocatalyst [(tbbpy)2Os(tpphz)PtI2](PF6)2 (tbbpy = 4,4′-tert-butyl-2,2′-bipyridine; tpphz = tetrapyrido[3,2-a:2′,3′-c:2′′,3′′-h:2′′′,3′′′-j]phenazine) is synthesized in order to make use of the broader range of visible light absorption mitigated by the osmium center. In a first step, the activity of the complex for hydrogen evolution is investigated by evaluating the role of different electron donors (triethylamine (TEA), 1-benzyl-1,4-dihydronicotinamide (BNAH) and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]-imidazole (BIH)). The highest photocatalytic activity (TON(H2) of 59) was observed for BIH as the electron donor. UV-vis investigations during catalysis with 470 nm (LED) irradiation show the rise of an absorption band at around 600 nm during catalysis, which indicates the reduction of the bridging ligand. Interestingly, broadband light excitation with wavelengths >450 nm induces no catalytic behavior. An intra-ligand charge transfer transition within the reduced tpphz moiety is hypothesized in order to rationalize the breakdown of the catalysis by broad band excitation.

Graphical abstract: Synthesis and hydrogen evolving catalysis of a panchromatic photochemical molecular device

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Supplementary files

Article information


Submitted
16 May 2019
Accepted
01 Sep 2019
First published
05 Sep 2019

Sustainable Energy Fuels, 2020, Advance Article
Article type
Paper

Synthesis and hydrogen evolving catalysis of a panchromatic photochemical molecular device

J. Habermehl, D. Nauroozi, M. Martynow, Y. E. Vilk, R. Beranek, J. Guthmuller and S. Rau, Sustainable Energy Fuels, 2020, Advance Article , DOI: 10.1039/C9SE00304E

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