A Polymer with “Locked” Degradability: Superior Backbone Stability and Accessible Degradability Enabled by Mechanophore Installation,Journal of the American Chemical Society

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A Polymer with “Locked” Degradability: Superior Backbone Stability and Accessible Degradability Enabled by Mechanophore Installation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-01-15 , DOI: 10.1021/jacs.9b12482
Tze-Gang Hsu ₁ , Junfeng Zhou ₁ , Hsin-Wei Su ₁ , Briana R Schrage ₂ , Christopher J Ziegler ₂ , Junpeng Wang ₁

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Though numerous applications require degradable polymers, there are surprisingly few polymer systems that combine superior stability and controllable degradability. Particularly, the degradability of a conventional degradable polymer is typically enabled by cleavable groups on the backbone, which can be attacked by stimuli in ambient conditions, causing undesirable material deterioration. Here we report a general strategy to overcome this issue: "locking" the degradability during handling and use of the polymers and "unlocking" it when degradation is needed. This strategy is demonstrated with a cyclobutane-fused lactone (CBL) polymer. The cyclobutane keeps the polymer backbone intact under conditions that hydrolyze the lactones and allows the ester group to be recovered when undesirable hydrolysis occurs. When backbone degradation is needed, the degradability can be unlocked by mechanochemical activation that converts the polyCBL into a linear polyester. The rare combination of two intrinsically conflicting properties, i.e., backbone stability and accessible degradability, can make this polymer an appealing choice for new sustainable materials.

中文翻译：

具有“锁定”降解性的聚合物：通过机械载体安装实现卓越的骨架稳定性和可降解性

尽管许多应用需要可降解聚合物，但令人惊讶的是，结合卓越稳定性和可控降解性的聚合物系统却很少。特别是，传统的可降解聚合物的可降解性通常是通过主链上的可裂解基团实现的，该基团可能会受到环境条件下的刺激的攻击，从而导致不希望的材料劣化。在这里，我们报告了克服这个问题的一般策略：在聚合物的处理和使用过程中“锁定”可降解性，并在需要降解时“解锁”它。这种策略是用环丁烷稠合内酯 (CBL) 聚合物证明的。环丁烷在水解内酯的条件下保持聚合物主链完整，并在发生不希望的水解时使酯基团得以恢复。当需要降解主链时，可通过机械化学活化将 polyCBL 转化为线性聚酯来解锁可降解性。两种本质上相互冲突的特性的罕见组合，即骨架稳定性和可降解性，可以使这种聚合物成为新型可持续材料的有吸引力的选择。

更新日期：2020-01-15

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