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

该奖项的全部或部分资金来自《2021年美国救援计划法案》(公共法律117-2)。在化学系化学催化项目的支持下，布朗大学的杰罗姆·罗宾逊和他的研究团队正在研究从廉价和丰富的材料中制造可生物降解塑料(聚合物)的新方法。聚合物使现代生活的几乎方方面面都取得了重大进展；然而，大多数聚合物最终进入了垃圾填埋场和水道，并需要几代人的时间才能在环境中降解。与目前具有环境持久性的合成材料相比，可持续替代材料的成本更高，性能更差，这限制了可持续替代材料的发展，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，用于构建生物可降解聚合物，并严格控制其分子结构和组成。拟议的研究具有重大的更广泛的社会影响，因为这种方法可以获得可扩展和负担得起的下一代材料，具有更好的性能和降解特征。罗宾逊博士和他的团队还在为高中、本科生和研究生开发项目，旨在培训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，将化学研究直接整合到罗德岛公立高中的体验中。其他教育和推广项目旨在提高该地区学生的教育公平，包括改善获得早期研究经验和职业职业发展的机会。在化学系化学催化项目的支持下，布朗大学的杰罗姆·罗宾逊和他的研究团队正在开发捐赠者放大的催化方法，用于立体控制的生物降解聚合物。调节不稳定的外源供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。Robinson小组的机械驱动实验和理论研究有望促进对如何利用施主效应来调节立体定向开环聚合(ROP)中催化剂性能的基本理解。预计这将使人们能够以立体控制的方式获得可生物降解的聚合物，包括那些从廉价和丰富的原料中提取的单体。这种化学作用应该导致可扩展和可持续的替代传统的、大容量的和环境持久的材料。罗宾逊博士的研究目标与专注于培训和指导多样化的STEM劳动力的教育目标紧密结合在一起。这包括与罗德岛州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，以及加强学生获得职业专业发展的机会。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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.