SusChEM: Resourceful Polymers Derived from Polyhydroxyl Natural Products

在这个由化学系高分子、超分子和纳米化学项目资助的项目中，德克萨斯农工大学的Karen Wooley教授正在研究如何从天然糖中合成复杂的聚合物。聚合物是一种长链有机分子，存在于日常生活的许多方面，使用塑料，包括食品包装、汽车和航空航天运输的结构材料，以及轻型电子设备。由天然化合物衍生的聚合物有望降解成完全生物兼容的产品。这项工作具有重要的科学和社会意义，原因如下：(1)减少我们对石油化工原料的依赖；(2)提高与合成先进聚合物材料有关的化学知识和实验技术；(3)产生可用作独特“塑料”的聚合物；(4)聚合物降解后产生环境可再吸收和生物有益(如营养、促生长、抗癌、抗炎或其他反应)产品。研究项目涉及合成化学方法的开发，目标是从可再生资源中生产一系列聚碳酸酯和聚磷酸酯，这些产品具有新颖的化学、物理和机械性能，并可被水解性分解为生物有益或良性的副产品。功能单体是由多羟基天然产物(主要是以糖为起始原料)制备的，并通过开环聚合转化。在一个方向上，正在制备环状碳酸酯单体，以产生含有碳酸酯键的聚合物。水解性降解会产生多羟基化合物和二氧化碳。在第二个方向上，正在利用从DNA或RNA等天然聚合物借来的磷酸酯键。正在进行研究，以促进环状碳酸酯或磷酸酯的受控开环聚合，以提供这些聚合物作为明确定义的大分子结构。聚合物的物理、机械和稳定性性能通过严格的物理化学和机械表征研究进行表征，并通过其化学组成和结构进行调整。该项目的更广泛影响涉及合成化学进展、开发的最终材料，以及参与拟议工作的学生和博士后同事的教育成果。该项目将科学和工程学院的研究和教育结合在一起。拟议的基于多羟基天然产物的聚碳酸酯有望展示出允许它们在解决现实世界问题的应用中开发的特性。

In this project funded by the Macromolecular, Supramolecular, and Nanochemistry Program of the Chemistry Division, Professor Karen Wooley of Texas A&M University is studying how to synthesize complex polymers from naturally occurring sugars. Polymers are long chain organic molecules and are found in many facets of everyday life that utilize plastics, including food packaging, structural materials for automotive and aerospace transportation, and lightweight electronic devices. Polymers derived from naturally occurring compounds are anticipated to degrade into completely biocompatible products. This work is of scientific and societal importance for several reasons, as it is expected to: (1) reduce our reliance on petrochemical feedstocks; (2) advance chemical knowledge and experimental techniques involved with the synthesis of advanced polymer materials; (3) generate polymers that will be useful as unique "plastics"; (4) produce environmentally-resorbable and biologically-beneficial (e.g., nutrient, growth-promoting, anti-cancer, anti-inflammatory or other responses) products upon degradation of the polymers.The research project involves the development of synthetic chemistry approaches with the objective being the production of a series of polycarbonates and polyphosphoesters that originate from renewable resources, exhibit novel chemical, physical and mechanical properties, and undergo hydrolytic breakdown to biologically-beneficial or benign by-products. Functional monomers are being prepared from polyhydroxyl natural products (as the primary focus, sugars are serving as the starting materials) and transformed by ring-opening polymerizations. In one direction, cyclic carbonate monomers are being prepared that will yield polymers that contain carbonate linkages. Hydrolytic degradation will produce the polyhydroxyl compound plus carbon dioxide. In a second direction, phosphoester linkages are being utilized, borrowing from natural polymers such as DNA or RNA. Studies are being performed to advance controlled ring opening polymerizations of cyclic carbonates or phosphoesters to afford these polymers as well-defined macromolecular structures. The physical, mechanical and stability properties of the polymers are being characterized using rigorous physicochemical and mechanical characterization studies and tuned via their chemical compositions and structures. The broader impacts of the project involve the synthetic chemistry advances, the ultimate materials that are developed, and the educational outcomes for the students and postdoctoral associates involved in the proposed work. The project integrates research and education across the schools of science and engineering. The proposed polyhydroxyl natural product-based polycarbonates are expected to exhibit properties that will allow for their development in applications that will solve real-world problems.