Clean Donor Oxidation Enhances the H2 Evolution Activity of a Carbon Quantum Dot-Molecular Catalyst Photosystem

Benjamin C M Martindale; Evelyne Joliat; Cyril Bachmann; Roger Alberto; Erwin Reisner

doi:10.1002/anie.201604355

Clean Donor Oxidation Enhances the H2 Evolution Activity of a Carbon Quantum Dot-Molecular Catalyst Photosystem

Angew Chem Int Ed Engl. 2016 Aug 1;55(32):9402-6. doi: 10.1002/anie.201604355. Epub 2016 Jun 29.

Authors

Benjamin C M Martindale¹, Evelyne Joliat², Cyril Bachmann², Roger Alberto², Erwin Reisner³

Affiliations

¹ Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.
² Department of Chemistry, University of Zürich, Winterthurerstrasse 190, 8057, Zürich, Switzerland.
³ Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK. reisner@ch.cam.ac.uk.

PMID: 27355200
DOI: 10.1002/anie.201604355

Abstract

Carbon quantum dots (CQDs) are new-generation light absorbers for photocatalytic H2 evolution in aqueous solution, but the performance of CQD-molecular catalyst systems is currently limited by the decomposition of the molecular component. Clean oxidation of the electron donor by donor recycling prevents the formation of destructive radical species and non-innocent oxidation products. This approach allowed a CQD-molecular nickel bis(diphosphine) photocatalyst system to reach a benchmark lifetime of more than 5 days and a record turnover number of 1094±61 molH2 (molNi )(-1) for a defined synthetic molecular nickel catalyst in purely aqueous solution under AM1.5G solar irradiation.

Keywords: carbon quantum dots; hydrogen evolution; molecular catalysis; photocatalysis; photosensitizers.

Publication types

Research Support, Non-U.S. Gov't