Design, synthesis, and characterization of vinyl-addition polynorbornenes with tunable thermal properties
Design, synthesis, and characterization of vinyl-addition polynorbornenes with tunable thermal properties
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具有可调热性能的乙烯基加成聚降冰片烯的设计、合成和表征
DOI：
10.1039/d1py01050f
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发表时间：
2021
影响因子：
4.6
通讯作者：
Long, Brian K.
中科院分区：
文献类型：
--
作者：
Wang, Xinyi;Jeong, Yewon L.;Love, Christopher;Stretz, Holly A.;Stein, Gila E.;Long, Brian K.
非官能化乙烯基加成聚异戊二烯（VAPNB）具有许多优异的性能，如高的热稳定性、化学稳定性和氧化稳定性。这些特性使VAPNB成为许多工程应用的有希望的候选者。然而，VAPNB在其玻璃化转变温度（Tg）和分解温度（Td）之间具有小的服务窗口，并且其不能容易地在熔融状态下加工。在这项工作中，我们证明了服务窗口的VAPNBs可以通过使用的顺丁烯单体轴承烷基，芳基和芳基醚取代基进行定制。这些官能化的丙烯基单体的乙烯基加成均聚和共聚产生具有高T′gs（>150 °C）和大服务窗口（Td-Tg > 100 °C）的VAPNB，其与其他商业工程热塑性塑料相当。为了进一步确立熔融加工的可行性，成功地挤出Tg = 209 °C和服务窗口为170 °C的官能化VAPNB材料并将其模制成条。随后通过动态力学分析（DMA）、核磁共振光谱（NMR）和凝胶渗透色谱（GPC）对棒进行表征，结果显示聚合物降解的迹象很小。这些研究表明，替代的VAPNB可以开发成一类新的工程热塑性塑料，与挤出和注塑等主力熔融加工技术以及基于挤出的3D打印等新兴技术兼容。
Unfunctionalized vinyl-addition polynorbornene (VAPNB) possesses many outstanding properties such as high thermal, chemical, and oxidative stability. These features make VAPNB a promising candidate for many engineering applications. However, VAPNB has a small service window between its glass transition temperature (Tg) and decomposition temperature (Td), and it cannot be readily processed in a melt state. In this work, we demonstrate that the service window of VAPNBs can be tailored through the use of norbornene monomers bearing alkyl, aryl, and aryl ether substituents. The vinyl addition homopolymerization and copolymerization of these functionalized norbornyl-based monomers yielded VAPNBs with high T′gs (>150 °C) and large service windows (Td–Tg > 100 °C), which are comparable to other commercial engineering thermoplastics. To further establish the feasibility of melt processing, a functionalized VAPNB material with Tg = 209 °C and a service window of 170 °C was successfully extruded and molded into bars. Subsequent characterization of the bars by dynamic mechanical analysis (DMA), nuclear magnetic resonance spectroscopy (NMR), and gel permeation chromatography (GPC) revealed only minor signs of polymer degradation. These studies suggest that substituted VAPNBs could be developed into a new class of engineering thermoplastics that is compatible with workhorse melt processing techniques such as extrusion and injection molding, as well as emerging techniques such as extrusion-based 3D printing.
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