Influence of monomer concentration on structures of fully condensed polyphenylsilsesquioxanes

IF 1.8 4区化学 Q3 POLYMER SCIENCE

High Performance Polymers Pub Date : 2023-12-18 DOI:10.1177/09540083231222593

Xiaolu Wu, Zhaolu Qin, Wenchao Zhang, Rongjie Yang

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引用次数: 0

Abstract

Fully condensed polyphenylsilsesquioxanes have been prepared via the hydrolysis and condensation of the same phenyltrimethoxysilane (PTMS) monomer in different concentrations. The effect of monomer concentration on molecular structure of the final products has been thoroughly investigated. Cage structured polyphenylsilsesquioxane (OPS) and ladder-like structured polyphenylsilsesquioxane (L-PPSQ) can be selectively synthesized from the same starting materials at lower and higher initial monomer concentrations. Meanwhile, online infrared detector, React IR TM15 was used to monitor the real time variation of the concentration and characteristic absorption peaks of any intermediate products that may exist. Then, React IR TM15 coupled with 29Si nuclear magnetic resonance spectroscopy (NMR), gel permeation chromatography (GPC) and matrix-assisted laser desorption/ionization-time of flight mass spectrometry (MALDI-TOF-MS) were used to monitor and identify the intermediate species during the reaction. Mechanism studies indicated that the condensation reaction of OPS and L-PPSQ both proceed through a T1 structure dimer, which was formed by the quick hydrolysis of the PTMS monomer. As confirmed by 29Si-NMR, GPC and MALDI-TOF-MS, the synthesis mechanisms of OPS and L-PPSQ during the hydrolysis-condensation reactions were delineated.

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单体浓度对完全缩合聚苯基硅倍半氧烷结构的影响

通过水解和缩合不同浓度的相同苯基三甲氧基硅烷（PTMS）单体，制备出了完全缩合的聚苯基硅倍半氧烷。我们深入研究了单体浓度对最终产品分子结构的影响。笼状结构聚苯基硅倍半氧烷（OPS）和阶梯状结构聚苯基硅倍半氧烷（L-PPSQ）可以在较低和较高的初始单体浓度下从相同的起始原料中选择性地合成。同时，在线红外检测器 React IR TM15 用于实时监测任何可能存在的中间产物的浓度变化和特征吸收峰。然后，React IR TM15 与 29Si 核磁共振波谱（NMR）、凝胶渗透色谱（GPC）和基质辅助激光解吸/电离飞行时间质谱（MALDI-TOF-MS）相结合，用于监测和鉴定反应过程中的中间产物。机理研究表明，OPS 和 L-PPSQ 的缩合反应都是通过 T1 结构二聚体进行的，该二聚体是由 PTMS 单体快速水解形成的。通过 29Si-NMR、GPC 和 MALDI-TOF-MS 的证实，阐明了 OPS 和 L-PPSQ 在水解缩合反应中的合成机理。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

High Performance Polymers 化学-高分子科学

CiteScore

4.20

自引率

14.30%

发文量

106

审稿时长

1.2 months

期刊介绍： Health Services Management Research (HSMR) is an authoritative international peer-reviewed journal which publishes theoretically and empirically rigorous research on questions of enduring interest to health-care organizations and systems throughout the world. Examining the real issues confronting health services management, it provides an independent view and cutting edge evidence-based research to guide policy-making and management decision-making. HSMR aims to be a forum serving an international community of academics and researchers on the one hand and healthcare managers, executives, policymakers and clinicians and all health professionals on the other. HSMR wants to make a substantial contribution to both research and managerial practice, with particular emphasis placed on publishing studies which offer actionable findings and on promoting knowledge mobilisation toward theoretical advances. All papers are expected to be of interest and relevance to an international audience. HSMR aims at enhance communication between academics and practitioners concerned with developing, implementing, and analysing health management issues, reforms and innovations primarily in European health systems and in all countries with developed health systems. Papers can report research undertaken in a single country, but they need to locate and explain their findings in an international context, and in international literature.