Dataset Information

Photoswitchable Sol-Gel Transitions and Catalysis Mediated by Polymer Networks with Coumarin-Decorated Cu₂₄ L₂₄ Metal-Organic Cages as Junctions.

ABSTRACT: Photoresponsive materials that change in response to light have been studied for a range of applications. These materials are often metastable during irradiation, returning to their pre-irradiated state after removal of the light source. Herein, we report a polymer gel comprising poly(ethylene glycol) star polymers linked by Cu₂₄ L₂₄ metal-organic cages/polyhedra (MOCs) with coumarin ligands. In the presence of UV light, a photosensitizer, and a hydrogen donor, this "polyMOC" material can be reversibly switched between Cu^II , Cu^I , and Cu⁰ . The instability of the MOC junctions in the Cu^I and Cu⁰ states leads to network disassembly, forming Cu^I /Cu⁰ solutions, respectively, that are stable until re-oxidation to Cu^II and supramolecular gelation. This reversible disassembly of the polyMOC network can occur in the presence of a fixed covalent second network generated in?situ by copper-catalyzed azide-alkyne cycloaddition (CuAAC), providing interpenetrating supramolecular and covalent networks.

SUBMITTER: Oldenhuis NJ

PROVIDER: S-EPMC7187918 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Publications

Photoswitchable Sol-Gel Transitions and Catalysis Mediated by Polymer Networks with Coumarin-Decorated Cu24 L24 Metal-Organic Cages as Junctions.

Oldenhuis Nathan J NJ Qin K Peter KP Wang Shu S Ye Hong-Zhou HZ Alt Eric A EA Willard Adam P AP Van Voorhis Troy T Craig Stephen L SL Johnson Jeremiah A JA

Angewandte Chemie (International ed. in English) 20200116 7

Photoresponsive materials that change in response to light have been studied for a range of applications. These materials are often metastable during irradiation, returning to their pre-irradiated state after removal of the light source. Herein, we report a polymer gel comprising poly(ethylene glycol) star polymers linked by Cu24 L24 metal-organic cages/polyhedra (MOCs) with coumarin ligands. In the presence of UV light, a photosensitizer, and a hydrogen donor, this "polyMO ...[more]

PMID: 31742840

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Project description:Titanium dioxide (TiO2) in the form of thin films has attracted enormous attention for photocatalysis. It combines the fundamental properties of TiO2 as a large bandgap semiconductor with the advantage of thin films, making it competitive with TiO2 powders for recycling and maintenance in photocatalytic applications. There are many aspects affecting the photocatalytic performance of thin film structures, such as the nanocrystalline size, surface morphology, and phase composition. However, the quantification of each influencing aspect needs to be better studied and correlated. Here, we prepared a series of TiO2 thin films using a sol-gel process and spin-coated on p-type, (100)-oriented silicon substrates with a native oxide layer. The as-deposited TiO2 thin films were then annealed at different temperatures from 400 °C to 800 °C for 3 h in an ambient atmosphere. This sample synthesis provided systemic parameter variation regarding the aspects mentioned above. To characterize thin films, several techniques were used. Spectroscopic ellipsometry (SE) was employed for the investigation of the film thickness and the optical properties. The results revealed that an increasing annealing temperature reduced the film thickness with an increase in the refractive index. Atomic force microscopy (AFM) was utilized to examine the surface morphology, revealing an increased surface roughness and grain sizes. X-ray diffractometry (XRD) and UV-Raman spectroscopy were used to study the phase composition and crystallite size. The annealing process initially led to the formation of pure anatase, followed by a transformation from anatase to rutile as the annealing temperature increased. An overall enhancement in crystallinity was also observed. The photocatalytic properties of the thin films were tested using the photocatalytic decomposition of acetone gas in a home-built solid (photocatalyst)-gas (reactant) reactor. The composition of the gas mixture in the reaction chamber was monitored using in situ Fourier transform infrared spectroscopy. Finally, all of the structural and spectroscopic characteristics of the TiO2 thin films were quantified and correlated with their photocatalytic properties using a correlation matrix. This provided a good overview of which film properties affect the photocatalytic efficiency the most.

Dataset Information

Photoswitchable Sol-Gel Transitions and Catalysis Mediated by Polymer Networks with Coumarin-Decorated Cu₂₄ L₂₄ Metal-Organic Cages as Junctions.

Publications

Photoswitchable Sol-Gel Transitions and Catalysis Mediated by Polymer Networks with Coumarin-Decorated Cu<sub>24</sub> L<sub>24</sub> Metal-Organic Cages as Junctions.

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