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Colloidally Stable CdS Quantum Dots in Water with Electrostatically Stabilized Weak-Binding, Sulfur-Free Ligands.

ABSTRACT: 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.

SUBMITTER: Arcudi F

PROVIDER: S-EPMC6854302 | biostudies-literature | 2019 Nov

REPOSITORIES: biostudies-literature

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Colloidally Stable CdS Quantum Dots in Water with Electrostatically Stabilized Weak-Binding, Sulfur-Free Ligands.

Arcudi Francesca F Westmoreland Dana Emily DE Weiss Emily Allyn EA

Chemistry (Weinheim an der Bergstrasse, Germany) 20191015 63

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, wh ...[more]

PMID: 31486120

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Project description:Previously we reported the biosynthesis of intracellular cadmium sulfide quantum dots (CdS QDs) at low temperatures by the Antarctic strain Pseudomonas fragi GC01. Here we studied the role of volatile sulfur compounds (VSCs) in the biosynthesis of CdS QDs by P. fragi GC01. The biosynthesis of nanoparticles was evaluated in the presence of sulfate, sulfite, thiosulfate, sulfide, cysteine and methionine as sole sulfur sources. Intracellular biosynthesis occurred with all sulfur sources tested. However, extracellular biosynthesis was observed only in cultures amended with cysteine (Cys) and methionine (Met). Extracellular nanoparticles were characterized by dynamic light scattering, absorption and emission spectra, energy dispersive X-ray, atomic force microscopy, transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Purified QDs correspond to cubic nanocrystals of CdS with sizes between 2 and 16 nm. The analysis of VSCs revealed that P. fragi GC01 produced hydrogen sulfide (H2S), methanethiol (MeSH) and dimethyl sulfide (DMS) in the presence of sulfate, Met or Cys. Dimethyl disulfide (DMDS) was only detected in the presence of Met. Interestingly, MeSH was the main VSC produced in this condition. In addition, MeSH was the only VSC for which the concentration decreased in the presence of cadmium (Cd) of all the sulfur sources tested, suggesting that this gas interacts with Cd to form nanoparticles. The role of MeSH and DMS on Cds QDs biosynthesis was evaluated in two mutants of the Antarctic strain Pseudomonas deceptionensis M1T: megL - (unable to produce MeSH from Met) and mddA - (unable to generate DMS from MeSH). No biosynthesis of QDs was observed in the megL - strain, confirming the importance of MeSH in QD biosynthesis. In addition, the production of QDs in the mddA - strain was not affected, indicating that DMS is not a substrate for the biosynthesis of nanoparticles. Here, we confirm a link between MeSH production and CdS QDs biosynthesis when Met is used as sole sulfur source. This work represents the first report that directly associates the production of MeSH with the bacterial synthesis of QDs, thus revealing the importance of different VSCs in the biological generation of metal sulfide nanostructures.

Dataset Information

Colloidally Stable CdS Quantum Dots in Water with Electrostatically Stabilized Weak-Binding, Sulfur-Free Ligands.

Publications

Colloidally Stable CdS Quantum Dots in Water with Electrostatically Stabilized Weak-Binding, Sulfur-Free Ligands.

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