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Photocatalytic H2 production from water with rhenium and cobalt complexes


Probst, B; Guttentag, M; Rodenberg, A; Hamm, P; Alberto, R (2011). Photocatalytic H2 production from water with rhenium and cobalt complexes. Inorganic Chemistry, 50(8):3404-3412.

Abstract

Photocatalytic hydrogen production in pure water for three component systems using a series of rhenium-based photosensitizers (PS) and cobalt-based water reduction catalysts (WRC), with triethanolamine (TEOA) as an irreversible electron donor, is described. Besides the feasibility of this reaction in water, key findings are reductive quenching of the excited state of the PS by TEOA (k(q) = 5-8 × 10(7) M(-1) s(-1); Φ(cage) = 0.75) and subsequent transfer of an electron to the WRC (k(Co(III)) = 1.1 × 10(9) M(-1) s(-1)). Turnover numbers in rhenium (TON(Re), H/Re) above 500 were obtained, whereas TON(Co) (H(2)/Co) did not exceed 17. It is shown that the cobalt-based WRC limits long-term performance. Long-term performance critically depends on pH and the type of WRC used but is unaffected by the type of PS or the concentration of WRC. A quantum yield of 30% was obtained (H/photon).

Photocatalytic hydrogen production in pure water for three component systems using a series of rhenium-based photosensitizers (PS) and cobalt-based water reduction catalysts (WRC), with triethanolamine (TEOA) as an irreversible electron donor, is described. Besides the feasibility of this reaction in water, key findings are reductive quenching of the excited state of the PS by TEOA (k(q) = 5-8 × 10(7) M(-1) s(-1); Φ(cage) = 0.75) and subsequent transfer of an electron to the WRC (k(Co(III)) = 1.1 × 10(9) M(-1) s(-1)). Turnover numbers in rhenium (TON(Re), H/Re) above 500 were obtained, whereas TON(Co) (H(2)/Co) did not exceed 17. It is shown that the cobalt-based WRC limits long-term performance. Long-term performance critically depends on pH and the type of WRC used but is unaffected by the type of PS or the concentration of WRC. A quantum yield of 30% was obtained (H/photon).

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:2011
Deposited On:07 Mar 2012 16:52
Last Modified:05 Apr 2016 15:41
Publisher:American Chemical Society
ISSN:0020-1669
Additional Information:This document is the Accepted Manuscript version of a Published Work that appeared in final form in Inorganic Chemistry, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/ic102317u
Publisher DOI:10.1021/ic102317u
PubMed ID:21366324
Permanent URL: http://doi.org/10.5167/uzh-60369

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