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

该奖项全部或部分由2021年美国救援计划法案（公法117-2）资助。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，大多数聚合物最终都会进入垃圾填埋场和水道，并需要几代人才能在环境中降解。与目前的环境持久性合成材料相比，可持续替代品的开发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，用于构建可生物降解的聚合物，并严格控制其分子结构和组成。拟议的研究具有更广泛的社会影响，因为这些方法可以获得可扩展且负担得起的下一代材料，这些材料具有更好的性能和降解特性。罗宾逊博士和他的团队还为高中生、本科生和研究生开发了一些项目，旨在培养和指导未来多元化的STEM（科学、技术、工程和数学）劳动力。这包括罗得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得岛公立高中的经验。额外的教育和推广计划旨在提高整个地区学生的教育公平性，包括改善获得早期研究经验和职业专业发展的机会。在化学系化学催化计划的支持下，布朗大学的杰罗姆罗宾逊和他的研究团队正在开发立体控制生物降解聚合物的供体放大催化方法。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。罗宾逊小组的机械驱动的实验和理论研究预计将促进对如何利用供体效应来调节立体定向开环聚合（ROP）中的催化剂性能的基本理解。预期这将使得能够立体控制地获得可生物降解的聚合物，包括衍生自单体的那些聚合物，所述单体本身源自廉价且丰富的原料。 这种化学反应应该导致可扩展和可持续的替代传统，大批量和环境持久性材料。罗宾逊博士的研究目标与专注于培训和指导多元化STEM劳动力的教育目标紧密结合。这包括与罗得岛公立高中的可持续课堂和研究合作伙伴关系，高中和本科生的早期研究经验，以及增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，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

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.