Heuchan Spencer M, MacDonald Jarret P, Bauman Lukas A, Fan Bo, Henry Hugh A L, Gillies Elizabeth R
Department of Biology and Department of Chemistry and the Centre for Advanced Materials and Biomaterials Research, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B7, Canada.
Department of Chemical and Biochemical Engineering, The University of Western Ontario, 1151 Richmond Street, London, Ontario N6A 5B9, Canada.
ACS Omega. 2018 Dec 28;3(12):18603-18612. doi: 10.1021/acsomega.8b02826. eCollection 2018 Dec 31.
Polymeric coatings are commonly employed to alter surface properties. While some coatings are designed to remain stable over a prolonged period, in applications such as pharmaceuticals or fertilizers, the coating is designed to erode and reveal or release the underlying material. Self-immolative polymers (SIPs) undergo depolymerization following the cleavage of stimuli-responsive end-caps from their termini, enabling controlled depolymerization in the solid state and in solution. Poly(ethyl glyoxylate) (PEtG) is a promising SIP because of its depolymerization to benign products, but its amorphous structure and low glass-transition temperature make it unsuitable alone for coating applications. This study explored the blending of PEtG with polyesters including polycaprolactone (PCL), poly(l-lactic acid), and poly(-3-hydroxybutyrate). Block copolymers of PEtG with PCL were also synthesized and studied. It was found that the phase separation behavior and consequently the thermal and mechanical properties of the materials could be tuned according to the composition of the blend, while the stimuli-responsive degradation of PEtG was retained in the blends. This work therefore provides a framework for the application of PEtG-based coatings in applications ranging from pharmaceuticals to agricultural products.
聚合物涂层通常用于改变表面性质。虽然有些涂层设计为在较长时间内保持稳定,但在制药或肥料等应用中,涂层的设计目的是侵蚀并露出或释放底层材料。自牺牲聚合物(SIPs)在其末端的刺激响应性封端被裂解后会发生解聚,从而能够在固态和溶液中进行可控解聚。聚乙醛酸乙酯(PEtG)因其解聚为良性产物而成为一种有前景的SIP,但它的无定形结构和低玻璃化转变温度使其单独不适用于涂层应用。本研究探索了PEtG与聚酯(包括聚己内酯(PCL)、聚(L-乳酸)和聚(-3-羟基丁酸酯))的共混。还合成并研究了PEtG与PCL的嵌段共聚物。研究发现,材料的相分离行为以及由此产生的热性能和机械性能可以根据共混物的组成进行调节,而PEtG的刺激响应性降解在共混物中得以保留。因此,这项工作为基于PEtG的涂层在从药品到农产品等各种应用中的应用提供了一个框架。