Header

UZH-Logo

Maintenance Infos

General scheme for oxidative quenching of a copper bis-phenanthroline photosensitizer for light-driven hydrogen production


Windisch, Johannes; Orazietti, Margherita; Hamm, Peter; Alberto, Roger; Probst, Benjamin (2016). General scheme for oxidative quenching of a copper bis-phenanthroline photosensitizer for light-driven hydrogen production. ChemSusChem, 9(13):1719-1726.

Abstract

A new, general reaction scheme for photocatalytic hydrogen production is presented based on oxidative quenching of a homoleptic copper(I) bis-1,10-phenanthroline photosensitizer (PS) by 1-methyl-4-phenyl-pyridinium (MPP(+) ) as the electron relay and subsequent regeneration of the so formed copper(II) complex by a sacrificial electron donor. Electron transfer from the relay to various cobalt based water reduction catalysts and subsequent H2 production was shown to close the catalytic cycle. Transient absorption experiments unambiguously confirmed the proposed pathway, both the oxidative quenching and subsequent regeneration of oxidized PS. Photocatalytic test runs further confirmed the role of MPP(+) and up to 10 turnovers were achieved in the relay. The performance limiting factor of the system was shown to be the decomplexation of the copper PS. Quantum yields of the system were 0.03 for H2 production, but 0.6 for MPP(.) formation, clearly indicating that unproductive pathways still prevail.

Abstract

A new, general reaction scheme for photocatalytic hydrogen production is presented based on oxidative quenching of a homoleptic copper(I) bis-1,10-phenanthroline photosensitizer (PS) by 1-methyl-4-phenyl-pyridinium (MPP(+) ) as the electron relay and subsequent regeneration of the so formed copper(II) complex by a sacrificial electron donor. Electron transfer from the relay to various cobalt based water reduction catalysts and subsequent H2 production was shown to close the catalytic cycle. Transient absorption experiments unambiguously confirmed the proposed pathway, both the oxidative quenching and subsequent regeneration of oxidized PS. Photocatalytic test runs further confirmed the role of MPP(+) and up to 10 turnovers were achieved in the relay. The performance limiting factor of the system was shown to be the decomplexation of the copper PS. Quantum yields of the system were 0.03 for H2 production, but 0.6 for MPP(.) formation, clearly indicating that unproductive pathways still prevail.

Statistics

Citations

3 citations in Web of Science®
3 citations in Scopus®
Google Scholar™

Altmetrics

Downloads

1 download since deposited on 04 Aug 2016
1 download since 12 months
Detailed statistics

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:7 July 2016
Deposited On:04 Aug 2016 12:21
Last Modified:08 Dec 2017 20:04
Publisher:Wiley-VCH Verlag
ISSN:1864-5631
Publisher DOI:https://doi.org/10.1002/cssc.201600422
PubMed ID:27226427

Download