Rethinking Electronic Effects in Photochemical Hydrogen Evolution Using CuInS₂@ZnS Quantum Dots Sensitizers
Abstract
Molecular catalysts based on coordination complexes for the generation of hydrogen via photochemical water splitting exhibit a large versatility and tunability of the catalytic properties through chemical functionalization. In the present work, we report on light-driven hydrogen production in an aqueous solution using a series of cobalt polypyridine complexes as hydrogen evolving catalysts (HECs) in combination with CuInS₂@ZnS quantum dots (QDs) as sensitizers, and ascorbate as the electron donor. A peculiar trend in activity has been observed depending on the substituents present on the polypyridine ligand. This trend markedly differs from that previously recorded using [Ru(bpy)₃]²⁺ (where bpy = 2,2'-bipyridine) as the sensitizer and can be ascribed to different kinetically limiting pathways in the photochemical reaction (viz. protonation kinetics with the ruthenium chromophore, catalyst activation via electron transfer from the QDs in the present system). Hence, this work shows how the electronic effects on light-triggered molecular catalysis are not exclusive features of the catalyst unit but depend on the whole photochemical system.
Additional Information
This research was funded by the University of Ferrara (FIR2021) and by the Swiss National Foundation (Grant 200021 159716).Additional details
- PMCID
- PMC9735784
- Eprint ID
- 118631
- Resolver ID
- CaltechAUTHORS:20230103-818063100.34
- 200021_159716
- Swiss National Science Foundation (SNSF)
- FIR2021
- University of Ferrara
- Created
-
2023-02-03Created from EPrint's datestamp field
- Updated
-
2023-02-03Created from EPrint's last_modified field