Diverse Degradable Polymers from Versatile Ring-Opening Metathesis (Co)Polymerization of Electron-Rich Cyclic Olefins

富电子环烯烃的多功能开环复分解（共）聚合得到多种可降解聚合物

• 批准号: 2106511
• 负责人: Yan Xia
• 金额: $ 60万
• 依托单位: Stanford University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2025-08-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2106511&HistoricalAwards=false
• 关键词: Diverse; Degradable; Polymers; Versatile; Ring

With the support of the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry, Professor Yan Xia of Stanford University will develop new chemistry for generating new types of degradable plastics to address the grand end-of-life challenge of persistent plastics to the environment and human health. In 2018, 27 million tons of plastics were landfilled or released into the environment in the US and are nondegradable. New polymers that are strategically designed to be recycled, degraded, or depolymerized on demand are highly desirable for environmental sustainability as well as many technological and biomedical applications. This project integrates educational endeavors at several levels to raise the public awareness of plastic pollution and recycling, and recruit and cultivate pre-college students, especially underrepresented students in the Bay Area, for future STEM careers. The research also provides perfect examples to interface organic chemistry, polymer science, and sustainability in undergraduate and graduate curriculum.Ring-opening metathesis polymerization (ROMP) of cyclic alkenes is a widely used method to synthesize controlled functional polymers. Enol ethers with an electron-rich alkene have long been believed to deactivate the catalysts for ROMP and routinely used to quench the polymerization. But the Xia laboratory discovered surprisingly efficient ROMP of cyclic enol ethers and their copolymerization with strained cyclic alkenes, leading to new types of degradable polymers with acid labile backbones. This research project will explore the metathesis chemistry of electron-rich heteroatom-substituted cyclic alkenes and their copolymerization for the first time, and understand how the thermodynamic and kinetic parameters impact the control, microstructures, degradation profiles, and physical properties of the resulting degradable/depolymerizable polymers.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系高分子、超分子和纳米化学项目的支持下，斯坦福大学夏燕教授将开发新的化学方法来生产新型可降解塑料，以应对持久性塑料的报废对环境和人类健康带来的巨大挑战。 2018年，美国有2700万吨塑料被填埋或释放到环境中，且不可降解。战略性设计为按需回收、降解或解聚的新型聚合物对于环境可持续性以及许多技术和生物医学应用来说是非常理想的。该项目整合了多个层面的教育工作，以提高公众对塑料污染和回收的认识，并招募和培养大学预科学生，特别是湾区代表性不足的学生，为未来的 STEM 职业生涯做好准备。该研究还为本科生和研究生课程中有机化学、聚合物科学和可持续发展的接口提供了完美的例子。环烯烃的开环复分解聚合（ROMP）是一种广泛使用的合成受控功能聚合物的方法。长期以来，人们一直认为烯醇醚与富电子烯烃会使 ROMP 催化剂失活，并通常用于猝灭聚合反应。但夏实验室发现了令人惊讶的高效 ROMP 环烯醇醚及其与应变环烯烃的共聚，从而产生了具有酸不稳定主链的新型可降解聚合物。该研究项目将首次探索富电子杂原子取代环烯烃及其共聚的复分解化学，并了解热力学和动力学参数如何影响所得可降解/可解聚聚合物的控制、微观结构、降解曲线和物理性能。该奖项反映了 NSF 的法定使命，并被视为 值得通过使用基金会的智力优点和更广泛的影响审查标准进行评估来支持。

项目成果

A versatile approach for the synthesis of degradable polymers via controlled ring-opening metathesis copolymerization

• DOI: 10.1038/s41557-021-00810-2
• 发表时间: 2021-11-18
• 期刊: NATURE CHEMISTRY
• 影响因子: 21.8
• 作者: Feist, John D.;Lee, Daniel C.;Xia, Yan
• 通讯作者: Xia, Yan