Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 63, Pages 14469-14474Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201903908
Keywords
catalysis; ligand design; nanotechnology; quantum dots; water chemistry
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Funding
- National Institutes of Health [R21GM127919]
- NIH [1S10OD012016-01/1S10RR019071-01A1]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- State of Illinois
- International Institute for Nanotechnology (IIN)
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Colloidal quantum dot (QD) photocatalysts have the electrochemical and optical properties to be highly effective for a range of redox reactions. QDs are proven photo-redox catalysts for a variety of reactions in organic solvents but are less prominent for aqueous reactions. Aqueous QD photocatalysts require hydrophilic ligand shells that provide long-term colloidal stability but are not so tight-binding as to prevent catalytic substrates from accessing the QD surface. Common thiolate ligands, which also poison many co-catalysts and undergo photo-oxidative desorption, are therefore often not an option. This paper describes a framework for the design of water-solubilizing ligands that are in dynamic exchange on and off the QD surface, but still provide long-term colloidal stability to CdS QDs. The binding affinity and inter-ligand electrostatic interactions of a bifunctional ligand, aminoethyl phosphonic acid (AEP), are tuned with the pH of the dispersion. The key to colloidal stability is electrostatic stabilization of the monolayer. This work demonstrates a means of mimicking the stabilizing power of a thiolate-bound ligand with a zwitterionic tail group, but without the thiolate binding group.
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