Dataset Information

Preparation of Silicophosphate Alternating Hybrid Copolymers via Nonaqueous Acid-Base Reactions of Phosphoric Acid and Organo-Bridged Bis(chlorosilane).

ABSTRACT: A design of atomic and oligomer level structure in organic-inorganic hybrid materials is highly important for various applications. Nonaqueous acid-base reaction allows us to prepare silicophosphates with controlled inorganic networks (-(O-P-O-Si)n) at atomic level because phosphorous and silicon-based precursors can react directly, resulting in an alternating copolymer network. Organic functionalization in those materials has been realized so far by using organic-modified phosphorous acid and/or organo-chlorosilane as precursors. In the present study, silicophosphate oligomers exhibiting inorganic-organic hybrid chains of (-(O-P-O-Si-R-Si)n) (R: bridging organic functional groups), are prepared from phosphoric acid and organo-bridged bis(chlorosilane). The 1, 2-bis(chlorodimethylsilyl)ethane ((C2H4)(Me2SiCl)2) and 1, 4-bis(chlorodimethylsilyl)benzene ((C6H4)(Me2SiCl)2) were used as organo-bridged bis(chlorosilane). Different types of silicophosphate oligomers with different network structures and terminal groups (P-OH and/or Si-Cl) were prepared by changing the reaction temperature and molar ratio of precursors. The formation of low molecular weight oligomers of ring and cage morphologies (ring tetramer, cage pentamer, and ring hexamer) is suggested in the product prepared from phosphoric acid and (C6H4)(Me2SiCl)2 molecule at 150 °C. Those silicophosphate hybrid oligomers are expected to be used as building blocks of hybrid materials with well-defined network structures for desired functionalities.

SUBMITTER: Okada K

PROVIDER: S-EPMC6983256 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature

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Preparation of Silicophosphate Alternating Hybrid Copolymers via Nonaqueous Acid-Base Reactions of Phosphoric Acid and Organo-Bridged Bis(chlorosilane).

Okada Kenji K Takano Masanari M Tokudome Yasuaki Y Tokuda Yomei Y Takahashi Masahide M

Molecules (Basel, Switzerland) 20191228 1

A design of atomic and oligomer level structure in organic-inorganic hybrid materials is highly important for various applications. Nonaqueous acid-base reaction allows us to prepare silicophosphates with controlled inorganic networks (-(O-P-O-Si)<sub>n</sub>) at atomic level because phosphorous and silicon-based precursors can react directly, resulting in an alternating copolymer network. Organic functionalization in those materials has been realized so far by using organic-modified phosphorous ...[more]

PMID: 31905676

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Project description:The importance of noncovalent interactions in the realm of biological materials continues to inspire efforts to create artificial supramolecular polymeric architectures. These types of self-assembled materials hold great promise as environmentally stimuli-responsive materials because they are capable of adjusting their various structural parameters, such as chain length, architecture, conformation, and dynamics, to new surrounding environments upon exposure to appropriate external stimuli. Nevertheless, in spite of considerable advances in the area of responsive materials, it has proved challenging to create synthetic self-assembled materials that respond to highly disparate analytes and whose environmentally induced changes in structure can be followed directly through both various spectroscopic and X-ray diffraction analyses. Herein, we report a new set of artificial self-assembled materials obtained by simply mixing two appropriately chosen, heterocomplementary macrocyclic receptors, namely a tetrathiafulvalene-functionalized calix[4]pyrrole and a bis(dinitrophenyl)-meso-substituted calix[4]pyrrole. The resulting polymeric materials, stabilized by combination of donor-acceptor and hydrogen bonding interactions, undergo dynamic, reversible dual guest-dependent structural transformations upon exposure to two very different types of external chemical inputs, namely chloride anion and trinitrobenzene. The structure and dynamics of the copolymers and their analyte-dependent responsive behavior was established via single crystal X-ray crystallography, SEM, heterocomplementary isodesmic analysis, 1- and 2D NMR, and dynamic light scattering spectroscopies. Our results demonstrate the benefit of using designed heterocomplementary interactions of two functional macrocyclic receptors to create synthetic, self-assembled materials for the development of "smart" sensory materials that mimic the key biological attributes of multianalyte recognition and substrate-dependent multisignaling.

Dataset Information

Preparation of Silicophosphate Alternating Hybrid Copolymers via Nonaqueous Acid-Base Reactions of Phosphoric Acid and Organo-Bridged Bis(chlorosilane).

Publications

Preparation of Silicophosphate Alternating Hybrid Copolymers via Nonaqueous Acid-Base Reactions of Phosphoric Acid and Organo-Bridged Bis(chlorosilane).

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