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Rethinking Electronic Effects in Photochemical Hydrogen Evolution Using CuInS₂@ZnS Quantum Dots Sensitizers

Orlando, Antonio and Lucarini, Fiorella and Benazzi, Elisabetta and Droghetti, Federico and Ruggi, Albert and Natali, Mirco (2022) Rethinking Electronic Effects in Photochemical Hydrogen Evolution Using CuInS₂@ZnS Quantum Dots Sensitizers. Molecules, 27 (23). Art. No. 8277. ISSN 1420-3049. PMCID PMC9735784. doi:10.3390/molecules27238277. https://resolver.caltech.edu/CaltechAUTHORS:20230103-818063100.34

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.3390/molecules27238277DOIArticle
http://www.ncbi.nlm.nih.gov/pmc/articles/pmc9735784/PubMed CentralArticle
ORCID:
AuthorORCID
Orlando, Antonio0000-0002-4166-8117
Lucarini, Fiorella0000-0001-7308-4098
Benazzi, Elisabetta0000-0001-6756-3842
Ruggi, Albert0000-0003-2860-9080
Natali, Mirco0000-0002-6638-978X
Additional Information:This research was funded by the University of Ferrara (FIR2021) and by the Swiss National Foundation (Grant 200021 159716).
Funders:
Funding AgencyGrant Number
Swiss National Science Foundation (SNSF)200021_159716
University of FerraraFIR2021
Issue or Number:23
PubMed Central ID:PMC9735784
DOI:10.3390/molecules27238277
Record Number:CaltechAUTHORS:20230103-818063100.34
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20230103-818063100.34
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118631
Collection:CaltechAUTHORS
Deposited By: Research Services Depository
Deposited On:03 Feb 2023 21:31
Last Modified:03 Feb 2023 21:31

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