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Clean Donor Oxidation Enhances the H 2 Evolution Activity of a Carbon Quantum Dot–Molecular Catalyst Photosystem
Author(s) -
Martindale Benjamin C. M.,
Joliat Evelyne,
Bachmann Cyril,
Alberto Roger,
Reisner Erwin
Publication year - 2016
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201604355
Subject(s) - aqueous solution , catalysis , photocatalysis , photochemistry , quantum dot , nickel , decomposition , carbon fibers , electron donor , chemistry , artificial photosynthesis , materials science , nanotechnology , organic chemistry , composite number , composite material
Carbon quantum dots (CQDs) are new‐generation light absorbers for photocatalytic H 2 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 mol H2 (mol Ni ) −1 for a defined synthetic molecular nickel catalyst in purely aqueous solution under AM1.5G solar irradiation.