CAREER: CAS: Donor-Amplified Catalytic Approaches to Stereocontrolled Biodegradable Polymers

该奖项的全部或部分资金由《2021年美国救援计划法案》（公法117-2）提供。在化学系化学催化项目的支持下，布朗大学的杰罗姆·罗宾逊和他的研究小组正在研究用廉价和丰富的材料制造可生物降解塑料（聚合物）的新方法。聚合物几乎在现代生活的各个方面都取得了重大进展；然而，大多数最终都被填埋在垃圾填埋场和水道中，需要几代人的时间才能在环境中降解。与目前的环境持久性合成材料相比，可持续替代品的发展受到成本较高和性能较差的限制，需要新的方法来应对这一挑战。罗宾逊博士的团队正在开发创新的催化剂，用于生物可降解聚合物的构建，并严格控制其分子结构和组成。拟议的研究具有重要的更广泛的社会影响，因为这种方法可以获得具有改进性能和降解特性的可扩展和负担得起的下一代材料。罗宾逊博士和他的团队还在为高中生、本科生和研究生开发项目，旨在培养和指导未来多样化的STEM（科学、技术、工程和数学）劳动力。这包括罗德岛可持续化学伙伴关系（RI SCP）计划，该计划将创造机会，直接将化学研究融入罗德岛公立高中的经历。其他教育和推广项目旨在提高整个地区学生的教育公平，包括改善获得早期研究经验和职业发展的机会。在化学系化学催化项目的支持下，布朗大学的杰罗姆·罗宾逊和他的研究小组正在开发供体放大催化方法，以制备立体控制的可生物降解聚合物。调节不稳定的外相给体和催化剂之间的动态交换过程可以显著提高不对称催化和多相催化的性能，但这种方法在生物可降解聚合物的合成中受到的关注有限。罗宾逊小组的机械驱动实验和理论研究有望推进对如何利用供体效应来调整立体定向开环聚合（ROP）中催化剂性能的基本理解。这有望使立体控制获得生物可降解聚合物，包括那些来自单体的聚合物，它们本身来自廉价和丰富的原料。这种化学反应将带来可扩展和可持续的替代品，以取代传统的、大批量的、环保的材料。罗宾逊博士的研究目标与教育目标紧密结合，专注于培训和指导多样化的STEM劳动力。这包括与罗德岛州的公立高中建立可持续的课堂和研究伙伴关系，为高中生和本科生提供早期研究经验，并增强学生获得职业发展的机会。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

This award is funded in whole or in part under the America Rescue Plan Act of 2021 (Public Law 117-2).With the support of the Chemical Catalysis program in the Division of Chemistry, Jerome Robinson of Brown University and his team of researchers are investigating new approaches to make biodegradable plastics (polymers) from inexpensive and abundant materials. Polymers have enabled critical advances in nearly every aspect of modern life; however, the majority end up in landfills and waterways and take generations to degrade in the environment. The development of sustainable substitutes has been limited by their higher cost and poorer properties compared to current environmentally persistent synthetic materials, and requires new approaches to address this challenge. Dr. Robinson’s team is developing innovative catalysts to be deployed in the construction of biodegradable polymers and to rigorously control their molecular structure and composition. The proposed research has significant broader societal impact, as such approaches could access scalable and affordable next-generation materials with improved properties and degradation profiles. Dr. Robinson and his team are also developing programs for high school, undergraduate, and graduate students that are designed to train and mentor a diverse STEM (Science, Technology, Engineering and Mathematics) workforce of the future. This includes the Rhode Island Sustainable Chemistry Partnerships (RI SCP) program that will create opportunities to directly integrate chemistry research into Rhode Island public high school experiences. Additional educational and outreach programs aim to enhance educational equity for students throughout the region, including improved access to early-stage research experiences and career professional development.With the support of the Chemical Catalysis program in the Division of Chemistry, Jerome Robinson of Brown University and his team of researchers are developing donor-amplified catalytic approaches to stereocontrolled biodegradable polymers. Modulation of dynamic exchange processes between labile exogeneous donors and catalysts can dramatically enhance performance in asymmetric catalysis and heterogeneous catalysis, yet such approaches have received limited attention in the synthesis of biodegradable polymers. Mechanistically driven experimental and theoretical studies from the Robinson group are expected to advance the fundamental understanding of how donor effects can be exploited to tune catalyst performance in stereospecific ring-opening polymerization (ROP). This is expected to enable stereocontrolled access to biodegradable polymers, including those derived from monomers that themselves emanate from inexpensive and abundant feedstocks. This chemistry should lead to scalable and sustainable alternatives to traditional, high-volume, and environmentally persistent materials. Dr. Robinson’s research goals are strongly integrated with educational objectives focused on training and mentoring a diverse STEM workforce. This includes sustainable classroom and research partnerships with public high schools in Rhode Island, early-stage research experiences for high school and undergraduate students, and enhanced student access to career professional development.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.