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Molecular Control of Internal Crystallization and Photocatalytic Function in Supramolecular Nanostructures.

ABSTRACT: Supramolecular light-absorbing nanostructures are useful building blocks for the design of next-generation artificial photosynthetic systems. Development of such systems requires a detailed understanding of how molecular packing influences the material's optoelectronic properties. We describe a series of crystalline supramolecular nanostructures in which the substituents on their monomeric units strongly affects morphology, ordering kinetics, and exciton behavior. By designing constitutionally-isomeric perylene monoimide (PMI) amphiphiles, the effect of side chain sterics on nanostructure crystallization was studied. Molecules with short amine linked alkyl-tails rapidly crystallize upon dissolution in water, while bulkier tails require the addition of salt to screen electrostatic repulsion and annealing to drive crystallization. A PMI monomer bearing a 3-pentylamine tail was found to possess a unique structure that results in strongly red-shifted absorbance, indicative of charge-transfer exciton formation. This particular supramolecular structure was found to have an enhanced ability to photosensitize a thiomolybdate, [(NH4)2Mo3S13], catalyst to generate hydrogen gas.

SUBMITTER: Kazantsev RV

PROVIDER: S-EPMC6366635 | biostudies-literature | 2018 Jul

REPOSITORIES: biostudies-literature

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Molecular Control of Internal Crystallization and Photocatalytic Function in Supramolecular Nanostructures.

Kazantsev Roman V RV Dannenhoffer Adam A Aytun Taner T Harutyunyan Boris B Fairfield Daniel J DJ Bedzyk Michael J MJ Stupp Samuel I SI

Chem 20180503 7

Supramolecular light-absorbing nanostructures are useful building blocks for the design of next-generation artificial photosynthetic systems. Development of such systems requires a detailed understanding of how molecular packing influences the material's optoelectronic properties. We describe a series of crystalline supramolecular nanostructures in which the substituents on their monomeric units strongly affects morphology, ordering kinetics, and exciton behavior. By designing constitutionally-i ...[more]

PMID: 30740552

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Project description:Nanosized tin oxide was fabricated with a simple and cost-effective precipitation technique and was analyzed by performing x-ray powder diffraction (XRD), Fourier-transform infrared (FT-IR) spectroscopy, high-resolution transmission electron (HR-TEM) microscopy, energy-dispersive x-ray (EDX) and UV-Vis spectroscopy. The XRD results revealed that tin oxide particles possessed typical orthorhombic structure and exhibited improved crystallinity with annealing. Calcination at 250 °C produced predominantly orthorhombic SnO which transformed to SnO2 at higher temperatures of 500 and 750 °C. HRTEM and FESEM images showed existence of agglomeration within the particles of tin oxide. The absorption was found to increase up to a certain annealing temperature followed by a decrease, which was recorded via UV-Vis spectroscopy. The effect of annealing temperature on dye decomposition behavior of synthesized photocatalysts was studied. It was noted that annealing temperature affects the size of synthesized particles, band gap width and photoactivity of tin oxide. The sample prepared at 500 °C followed first-order kinetics and exhibited maximum photocatalytic reactivity toward methylene blue. The experimental results obtained from the present study indicate that SnO2 is a promising and beneficial catalyst to remove contaminants from wastewater and environment. The antimicrobial evaluation of SnO annealed at 500 °C against selected targets such as E. coli and S. aureus depicted significant inhibition zones in comparison with 250 and 750 °C samples. Furthermore, molecular docking predictions of SnO2 nanoparticles (NPs) were performed against active pocket of ?-lactamase and DNA gyrase enzyme belonging to cell wall and nucleic acid biosynthetic pathway, respectively. The fabricated NPs showed good binding score against ?-lactamase of both E. coli (-?5.71 kcal/mol) and S. aureus (-?11.83 kcal/mol) alongside DNA gyrase (-?9.57 kcal/mol; E. coli and -?8.61 kcal/mol; S. aureus). These in silico predictions suggested SnO2 NPs as potential inhibitors for selected protein targets and will facilitate to have a clear understanding of their mechanism of action that may contribute toward new antibiotics discovery.

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Molecular Control of Internal Crystallization and Photocatalytic Function in Supramolecular Nanostructures.

Publications

Molecular Control of Internal Crystallization and Photocatalytic Function in Supramolecular Nanostructures.

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