CAS: Synthetic Methodologies to Harness the Chemical Diversity of Natural Products for the Sustainable Production of High Value Macromolecular Materials

CAS：利用天然产物化学多样性实现高价值高分子材料可持续生产的合成方法

• 批准号: 2003771
• 负责人: Karen Wooley
• 金额: $ 70万
• 依托单位: Texas A&M University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-01 至 2025-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2003771&HistoricalAwards=false
• 关键词: CAS; Synthetic; Methodologies; Harness; Chemical

In this project funded by the Macromolecular, Supramolecular, and Nanochemistry Program in the Division of Chemistry, Professors Karen L. Wooley and Donald J. Darensbourg of the Department of Chemistry at Texas A&M University are developing new synthetic routes that harness natural products and consume carbon dioxide for the sustainable production of high value polymers. These polymers are capable of undergoing degradation to regenerate the same natural building blocks once they have completed their useful lifetime. The team quantifies the polymer degradation products and defines the potential uses of the polymers. The broader impacts of this research include the transformation of natural resources into useful polymer materials that can be readily and sustainably degraded, thereby reducing the use of petrochemical feedstocks and reducing the environmental persistence of plastics in landfills and water systems. The project also contributes to the training of a diverse group of students in a highly interdisciplinary research environment and is complemented by outreach activities and efforts at recruiting the next generation STEM workforce. This research is focused on developing synthetic chemistry approaches to the production of a series of polycarbonates, polyphosphoesters, polyamides and polyurethanes that originate from renewable resources. These materials exhibit novel chemical, physical and mechanical properties, and undergo hydrolytic breakdown to biologically-beneficial or benign by-products. Linkages between carbohydrate repeat units are designed to include carbonates to allow for breakdown to carbohydrates, carbon dioxide and other byproducts upon hydrolysis. To be carbon dioxide neutral, carbon dioxide is used as a feedstock to access the polycarbonates. Carbohydrates are also connected via phosphoesters, analogous to polyphosphoesters backbones in DNA. Polyphenolic compounds are investigated as alternatives to bisphenol A in the construction of engineering plastics or polyurethanes. Additionally, and of importance for polyurethane industry, several natural diamines and diols are studied for conversion into polyurethanes via processes that avoid phosgene and handing of isocyanates. Polymerizations associated with this work involve step-growth condensation or chain-growth ring opening polymerization. This work includes research and educational components that have a high potential to impact advanced manufacturing.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.

在该项目由大分子，超分子和纳米化学计划资助的项目中，得克萨斯州A＆M大学化学系的Karen L. Wooley和Donald J. Darensbourg教授正在开发新的合成路线，以利用自然产品和可持续生产高价值的Polymers consuty Naturals Production and Coarbon Doxide。 一旦完成有用的寿命，这些聚合物能够进行降解以再生相同的自然构件。 团队量化聚合物降解产品并定义了聚合物的潜在用途。 这项研究的更广泛的影响包括将自然资源转变为有用的聚合物材料，可以轻松降低，从而减少石化原料的使用并减少垃圾填埋场和水系统中塑料的环境持久性。 该项目还为在高度跨学科的研究环境中培训了一群学生，并得到了外展活动和招募下一代STEM劳动力的努力的补充。 这项研究的重点是开发合成化学方法来生产一系列源自可再生资源的聚碳酸酯，聚磷酸酯，聚酰胺和聚氨酯。 这些材料具有新颖的化学，物理和机械性能，并经历了水解分解为生物学或良性副产品。 碳水化合物重复单位之间的连锁旨在包括碳酸盐，以使水解后碳水化合物，二氧化碳和其他副产品分解。 为了二氧化碳中性，二氧化碳被用作进入聚碳酸酯的原料。 碳水化合物也通过磷酸植物连接，类似于DNA中的多磷酸酯骨架。 在工程塑料或聚氨酯构建中，研究了多酚化合物作为双酚A的替代方法。 此外，对聚氨酯工业的重要性很重要，还研究了几种天然二醇和二醇，以通过避免磷酸化和触发异氰酸酯的过程转换为聚氨酯。 与这项工作相关的聚合涉及级增长凝结或链生长环开放聚合。 这项工作包括具有影响高级制造业潜力的高潜力的研究和教育组成部分。该奖项反映了NSF的法定任务，并且使用基金会的知识分子优点和更广泛的影响审查标准，被认为值得通过评估来获得支持。

项目成果

Elucidation of Substantial Differences in Ring-Opening Polymerization Outcomes from Subtle Variation of Glucose Carbonate-Based Monomer Substitution Patterns and Substituent Types

• DOI: 10.1021/jacs.3c03339
• 发表时间: 2023-07
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Yidan Shen;Mingwan Leng;Yunchong Yang;Senthil K. Boopathi;Guorong Sun;K. Wooley

Design of nanoconstructs that exhibit enhanced hemostatic efficiency and bioabsorbability

• DOI: 10.1039/d2nr02043b
• 发表时间: 2022-07-22
• 期刊: NANOSCALE
• 影响因子: 6.7
• 作者: Eissa, Rana A.;Saafan, Hesham A.;Wooley, Karen L.
• 通讯作者: Wooley, Karen L.

Morphologic design of sugar-based polymer nanoparticles for delivery of antidiabetic peptides

• DOI: 10.1016/j.jconrel.2021.04.006
• 发表时间: 2021-04-18
• 期刊: JOURNAL OF CONTROLLED RELEASE
• 影响因子: 10.8
• 作者: Elsabahy, Mahmoud;Song, Yue;Wooley, Karen L.
• 通讯作者: Wooley, Karen L.

Polypeptide organic radical batteries

• DOI: 10.1038/s41586-021-03399-1
• 发表时间: 2021-05-06
• 期刊: NATURE
• 影响因子: 64.8
• 作者: Nguyen, Tan P.;Easley, Alexandra D.;Wooley, Karen L.
• 通讯作者: Wooley, Karen L.

A Tale of Drug-Carrier Optimization: Controlling Stimuli Sensitivity via Nanoparticle Hydrophobicity through Drug Loading

• DOI: 10.1021/acs.nanolett.0c02319
• 发表时间: 2020-09-09
• 期刊: NANO LETTERS
• 影响因子: 10.8
• 作者: Lin, Yen-Nan;Khan, Sarosh;Wooley, Karen L.
• 通讯作者: Wooley, Karen L.