Header

UZH-Logo

Maintenance Infos

Quinones as reversible electron relays in artificial photosynthesis


Rodenberg, Alexander; Orazietti, Margherita; Mosberger, Mathias; Bachmann, Cyril; Probst, Benjamin; Alberto, Roger; Hamm, Peter (2016). Quinones as reversible electron relays in artificial photosynthesis. ChemPhysChem, 17(9):1321-1328.

Abstract

We explore the potential of various hydroquinone/quinone redox couples as electron relays in a homogenous water reduction system between a Re-based photosensitizer and a sacrificial electron donor [tris-(2-carboxyethyl)-phosphine, TCEP]. By using transient IR spectroscopy, flash photolysis as well as stopped-flow techniques covering timescales from picoseconds to 100 ms, we determine quenching rates and cage escape yields, the kinetics of the follow-up chemistry of the semiquinone, the recombination rates, as well as the re-reduction rates by TCEP. The overall quantum yield of hydrogen production is low, and we show that the limiting factors are the small cage escape yields and, more importantly, the slow regeneration rate by TCEP in comparison to the undesired charge recombination with the reduced water reduction catalyst.

Abstract

We explore the potential of various hydroquinone/quinone redox couples as electron relays in a homogenous water reduction system between a Re-based photosensitizer and a sacrificial electron donor [tris-(2-carboxyethyl)-phosphine, TCEP]. By using transient IR spectroscopy, flash photolysis as well as stopped-flow techniques covering timescales from picoseconds to 100 ms, we determine quenching rates and cage escape yields, the kinetics of the follow-up chemistry of the semiquinone, the recombination rates, as well as the re-reduction rates by TCEP. The overall quantum yield of hydrogen production is low, and we show that the limiting factors are the small cage escape yields and, more importantly, the slow regeneration rate by TCEP in comparison to the undesired charge recombination with the reduced water reduction catalyst.

Statistics

Citations

Dimensions.ai Metrics
5 citations in Web of Science®
5 citations in Scopus®
4 citations in Microsoft Academic
Google Scholar™

Altmetrics

Downloads

0 downloads since deposited on 04 Aug 2016
0 downloads since 12 months

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:4 May 2016
Deposited On:04 Aug 2016 07:19
Last Modified:02 Feb 2018 10:12
Publisher:Wiley-Blackwell Publishing, Inc.
ISSN:1439-4235
OA Status:Closed
Publisher DOI:https://doi.org/10.1002/cphc.201501085
PubMed ID:26752324

Download