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Functional silanes are multifaceted cross-linkers, compatibilizers, coupling agents, and surface modifiers. Herein, we present organofunctional polysiloxane building blocks that offer great versatility in terms of molecular weight, degree of condensation, and the choice and loading of organic substituent groups. The organofunctional polyethoxysilanes (funPEOS) are prepared in a one-pot, two-step process: synthesis of the PEOS carrier/substrate, followed by grafting a functional silane "shell", both based on condensation with acetic anhydride. The reaction was optimized at the lab scale and scaled up to a 7 L reactor. The acetylation, condensation, and hyperbranched structure of the carrier were confirmed by Si NMR, while Si-Si 2D INADEQUATE NMR provides strong evidence for the grafting of functional silanes onto the carrier (Q-T coupling). IR, H, and C NMR spectroscopy demonstrate that the functional groups remain intact. The molar mass can be tailored by stoichiometric control of the acetic anhydride to silane monomer ratio ( 3500-20,000 g/mol). The compounds are stable organic liquids with a long shelf life. Selected applications are presented: scratch-resistant coatings with water contact angles of ∼90°, stable water emulsions, and surfactant-free, mesoporous silica foams.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11217919 | PMC |
http://dx.doi.org/10.1021/acsapm.4c00758 | DOI Listing |
J Am Chem Soc
December 2024
Univ Rennes, ENSCR, CNRS, ISCR-UMR6226, Université de Rennes, Rennes 35042, France.
Metal halide perovskites, including some of their related perovskitoid structures, form a semiconductor class of their own, which is arousing ever-growing interest from the scientific community. With halides being involved in the various structural arrangements, namely, pure corner-sharing MX (M is metal and X is halide) octahedra, for perovskite networks, or alternatively a combination of corner-, edge-, and/or face-sharing for related perovskitoids, they represent the ideal probe for characterizing the way octahedra are linked together. Well known for their inherently large quadrupolar constants, which is detrimental to the resolution of nuclear magnetic resonance spectroscopy, most abundant halide isotopes (Cl, Br, I) are in turn attractive for magnetic field-free nuclear quadrupolar resonance (NQR) spectroscopy.
View Article and Find Full Text PDFWe report on continuous high-harmonic generation (HHG) at 1 kHz repetition rate from a liquid-sheet plasma mirror driven by relativistic-intensity near-single-cycle light transients. Through precise control of both the surface plasma density gradient and the driving light waveform, we can produce highly stable and reproducible extreme ultraviolet spectral quasi-continua, expected to correspond to the generation of stable kHz-trains of isolated attosecond pulses in the time domain. This confirms the exciting potential of liquid-sheet targets as one of the building blocks of future high-power attosecond lasers.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Department of Chemistry at Brown University, 324 Brook Street, Providence, Rhode Island 02912, United States.
Biomacromolecular networks with multiscale fibrillar structures are characterized by exceptional mechanical properties, making them attractive architectures for synthetic materials. However, there is a dearth of synthetic polymeric building blocks capable of forming similarly structured networks. Bottlebrush polymers (BBPs) are anisotropic graft polymers with the potential to mimic and replace biomacromolecules such as tropocollagen for the fabrication of synthetic fibrillar networks; however, a longstanding limitation of BBPs has been the lack of rigidity necessary to access the lyotropic ordering that underpins the formation of collagenous networks.
View Article and Find Full Text PDFJ Org Chem
December 2024
Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, 1-13-27 Kasuga, Bunkyo-ku, Tokyo 112-8551, Japan.
(-)-Exiguolide is a marine macrolide natural product with potent anticancer activity. In this study, the total synthesis of exiguolide stereoisomers, (9)-exiguolide, (9,13)-exiguolide, and (9,13,19)-exiguolide, was achieved by capitalizing on our macrocyclization/transannular pyran cyclization strategy. The impact of the stereochemical permutation on the reactivity of advanced intermediates, the conformation of the macrocyclic skeleton, and the antiproliferative activity against human cancer cells were investigated in detail.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Northeast Forestry University, Key Laboratory of Bio-based Material Science and Technology of Ministry of Education, CHINA.
Materials with red room-temperature phosphorescence (RTP) derived from sustainable sources are crucial but rarely reported. Here, we produced red RTP materials from lignin. Lignin was covalently modified with Upy (1-(6-isocyanatohexyl)-3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl) urea) to obtain Lig-Upy.
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