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Switchable Catalysis as a tool for the Synthesis of Novel Multiblock Copolymers

可转换催化作为合成新型多嵌段共聚物的工具

基本信息

批准号：
1809116
负责人：
Paula Diaconescu
金额：
$ 80万
依托单位：
University of California-Los Angeles
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-08-15 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1809116&HistoricalAwards=false
关键词：
Switchable Catalysis tool Synthesis Novel

项目摘要

Polymers are large molecules that are made up of smaller molecules (monomers) linked together in a process called "polymerization". Polymers are found in nature, which has evolved complex machinery for controlling polymerization in a precise manner. While natural systems are limited to making polymers from only a few types of monomers, synthetic chemistry offers the opportunity to create polymers from an essentially infinite variety of monomers. These man-made polymers make up a wide range of materials. Man-made catalysts, however, cannot control monomer incorporation into a growing polymer to the degree that natural systems can. As such, methods that can achieve precise control of monomer incorporation and polymer structure are needed. Professor Diaconescu from University of California Los Angeles is designing metal catalysts that can exist in two states and can create different polymers in each of these states. By switching the state of the catalyst, the Diaconescu group can make different block copolymers (i.e., polymers that consist of a "block" of one monomer followed by another block made of different monomers). With this award from the Macromolecular, Supramolecular and Nanochemistry Program and the Chemical Catalysis Program, Professor Diaconescu is studying the design and reactivity of switchable catalysts and is applying the catalysts to the synthesis of new, biodegradable polymeric materials. These materials are excellent candidates for understanding the properties of multiblock copolymers. The project contributes to the development of human resources in science, technology, and engineering through the education of postdoctoral fellows, graduate students, undergraduates. This project is also providing summer research opportunities for high school students from the High School Nanoscience Program, a partnership between UCLA and the Los Angeles Unified School District, organized by California NanoSystems Institute.The Diaconescu group is studying the design and mechanism of action of redox switchable polymerization catalysts for the formation of biodegradable copolymers. Applications of the catalysts to the production of multiblock copolymers are also being pursued. The polymerization methods rely on metal catalysts capable of carrying out the redox switchable copolymerization of epoxides, lactide, lactones, and carbonates, monomers that are biocompatible, biodegradable, and nonimmunogenic. The group is using experimental and computational approaches, including quantitative structure-activity relationships (QSAR) guided by principal component analysis (PCA) to understand the mechanism and improve catalyst function. The properties of the generated materials are investigated with an emphasis on characterizing multi-compartment micelles and sequence-defined multiblock copolymers.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.

聚合物是由较小分子（单体）在称为“聚合”的过程中连接在一起组成的大分子。聚合物存在于自然界中，自然界已经进化出复杂的机制来以精确的方式控制聚合。虽然天然系统仅限于从几种类型的单体制造聚合物，但合成化学提供了从基本上无限种类的单体制造聚合物的机会。这些人造聚合物构成了各种各样的材料。然而，人造催化剂不能像自然系统那样控制单体掺入到生长的聚合物中。因此，需要能够实现单体掺入和聚合物结构的精确控制的方法。来自加州洛杉矶大学的Diaconescu教授正在设计可以存在于两种状态的金属催化剂，并可以在每种状态下产生不同的聚合物。通过切换催化剂的状态，Diaconescu基团可以制备不同的嵌段共聚物（即，由一种单体的“嵌段”接着由不同单体制成的另一嵌段组成的聚合物）。凭借大分子，超分子和纳米化学计划以及化学催化计划的这一奖项，Diaconescu教授正在研究可转换催化剂的设计和反应性，并将催化剂应用于新的可生物降解聚合物材料的合成。这些材料是理解多嵌段共聚物性质的极好候选材料。该项目通过博士后研究员、研究生和本科生的教育，为科学、技术和工程领域的人力资源开发做出贡献。该项目还为高中纳米科学项目的高中生提供暑期研究机会，该项目是加州大学洛杉矶分校和洛杉矶联合学区之间的合作伙伴关系，由加州纳米系统研究所组织。Diaconescu小组正在研究用于形成可生物降解共聚物的氧化还原可切换聚合催化剂的设计和作用机制。催化剂在多嵌段共聚物生产中的应用也在进行中。聚合方法依赖于能够进行环氧化物、丙交酯、内酯和碳酸酯的氧化还原可切换共聚的金属催化剂，这些单体是生物相容的、生物可降解的和非免疫原性的。该小组正在使用实验和计算方法，包括由主成分分析（PCA）指导的定量结构-活性关系（QSAR），以了解机制并改善催化剂功能。该奖项反映了NSF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。

项目成果

期刊论文数量（24）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Synthesis and Self-assembly of Limonene Oxide – Lactide Block Copolymers

氧化柠檬烯-丙交酯嵌段共聚物的合成与自组装

DOI：
发表时间：
2023
期刊：
ChemRxiv
影响因子：
0
作者：
Dai, Ruxi;Valloppilly, Shah;Watuthanthrige, Nethmi D.;Chakma, Progyateg;Deng, Shijie;Konkolewicz, Dominik;Diaconescu, Paula L.
通讯作者：
Diaconescu, Paula L.

Post-functionalization and Mechanical Properties of Poly(lactide-cyclohexadiene oxide) Block Copolymers

聚丙交酯-环己二烯氧化物嵌段共聚物的后官能化和机械性能

DOI：
发表时间：
2023
期刊：
ChemRxiv
影响因子：
0
作者：
Dai, Ruxi;Deng, Shijie;Peng, Zihang;Pei, Qibing;Diaconescu, Paula L.
通讯作者：
Diaconescu, Paula L.

Arene-Bridged Dithorium Complexes: Inverse Sandwiches Supported by a δ Bonding Interaction

芳烃桥二钍配合物：Î´ 键相互作用支持的反三明治

DOI：
10.1021/jacs.0c11215
发表时间：
2020
期刊：
Journal of the American Chemical Society
影响因子：
15
作者：
Yu, Chao;Liang, Jiefeng;Deng, Chong;Lefèvre, Guillaume;Cantat, Thibault;Diaconescu, Paula L.;Huang, Wenliang
通讯作者：
Huang, Wenliang

ABCD Block Copolymers Using a Multistate Aluminum Complex

使用多态铝配合物的 ABCD 嵌段共聚物

DOI：
发表时间：
2023
期刊：
ChemRxiv
影响因子：
0
作者：
Lin, Shiyun;Vasisht, Maya;Massad, Ramzi;Roshandel, Hootan;Wong, Yin-Pok;Diaconescu, Paula L.
通讯作者：
Diaconescu, Paula L.

ABC and ABAB Block Copolymers by Electrochemically Controlled Ring-Opening Polymerization