CAREER: Ribosome-inspired Synthesis of Precision Polymers

职业：核糖体启发的精密聚合物合成

• 批准号: 1848444
• 负责人: Severin Schneebeli
• 金额: $ 67.86万
• 依托单位: University of Vermont & State Agricultural College
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-07-01 至 2023-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1848444&HistoricalAwards=false
• 关键词: CAREER; Ribosome; inspired; Synthesis; Precision

Nature builds very large molecules (so called polymers) with molecular assembly lines. Crucial for life, these assembly lines add building blocks to growing polymer chains one after another in a specific order. This is how DNA and RNA are formed. In this project, Dr. Schneebeli is imitating the natural assembly-line approach to create well-defined polymeric materials. While this research focuses on enabling and understanding artificial molecular assembly lines, the well-defined polymers created may ultimately be useful materials for a variety of important applications. The artificial molecular assembly lines are created by connecting a catalyst to the polymers with rings that slide along the growing chains. This catalyst adds individual building blocks to the growing polymers one by one. In addition, Dr. Schneebeli is engaging the public in polymer chemistry through K-12 outreach at a local science museum (ECHO Lake Aquarium and Science Center in Burlington, VT) and at local high schools. For this outreach, Dr. Schneebeli is inventing interactive dynamic models. These models lead K-12 students to discover key aspects of polymer growth independently and foster independent creative thinking within the future STEM workforce.With support from the Chemical Catalysis Program of the Chemistry Division, Dr. Schneebeli of the University of Vermont is learning how to enable new polymerization mechanisms that could ultimately result in molecular assembly lines for sequence-defined, pi-conjugated polymers. Inspired by how Nature creates sequence-defined, functional macromolecules, Dr. Schneebeli is creating special interlocked catalysts, which can transform difficult-to-control step polymerizations into robust living chain-growth processes. While efficient chain-growth processes exist for numerous conjugated, cyclic, and hyperbranching monomers, this research explores a universal chain-growth strategy for general monomers, many of which cannot yet be polymerized in a controlled manner. Dr. Schneebeli's design prevents the catalysts from falling off the polymers, thus rendering this new living polymerization methodology fully chain-transfer free. Dr. Schneebeli is utilizing this new polymerization technique to enable the enzyme-free translation of DNA templates into diverse, pi-conjugated precision polymers, in a manner analogous to how the ribosome builds proteins. In support of the broader impacts of the project, Dr. Schneebeli is actively engaged in K-12 outreach with special macroscopic dynamic models. These models are devised to lead K-12 students to discover qualitative and quantitative aspects of different polymerization mechanisms to foster discovery-based reasoning and creative thinking among the future STEM workforce.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.

大自然用分子装配线制造出非常大的分子（所谓的聚合物）。这些装配线对生命至关重要，它们以特定的顺序为不断生长的聚合物链添加积木。DNA和RNA就是这样形成的。在这个项目中，Schneebeli博士正在模仿自然装配线的方法来创造定义良好的聚合物材料。虽然这项研究的重点是实现和理解人工分子装配线，但所创建的定义良好的聚合物最终可能成为各种重要应用的有用材料。人工分子装配线是通过将催化剂与沿着生长链滑动的环连接到聚合物上而形成的。这种催化剂将单个构建块一个接一个地添加到正在生长的聚合物中。此外，Schneebeli博士还通过当地科学博物馆（位于佛蒙特州伯灵顿的回声湖水族馆和科学中心）和当地高中的K-12外展活动，让公众参与到聚合物化学中来。为了推广，施尼贝利博士发明了互动动态模型。这些模型引导K-12学生独立发现聚合物生长的关键方面，并在未来的STEM劳动力中培养独立的创造性思维。在化学部化学催化项目的支持下，佛蒙特大学的Schneebeli博士正在学习如何实现新的聚合机制，从而最终形成序列定义的pi共轭聚合物的分子装配线。Schneebeli博士受到大自然创造序列定义的功能大分子的启发，正在创造特殊的连锁催化剂，可以将难以控制的步骤聚合转化为强大的生活链生长过程。虽然有效的链生长过程存在于许多共轭、环状和超分支单体中，但本研究探索了一般单体的普遍链生长策略，其中许多单体还不能以受控的方式聚合。Schneebeli博士的设计可以防止催化剂从聚合物上脱落，从而使这种新的活性聚合方法完全无链转移。Schneebeli博士正在利用这种新的聚合技术，以一种类似于核糖体构建蛋白质的方式，将DNA模板无酶翻译成各种pi共轭的精密聚合物。为了支持该项目更广泛的影响，Schneebeli博士积极参与K-12的推广活动，使用特殊的宏观动态模型。这些模型旨在引导K-12学生发现不同聚合机制的定性和定量方面，以培养未来STEM劳动力中基于发现的推理和创造性思维。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。

项目成果

Outcome-Based Redesign of Physical Chemistry Laboratories During the COVID-19 Pandemic

COVID-19 大流行期间物理化学实验室基于结果的重新设计

• DOI: 10.1021/acs.jchemed.1c00691
• 发表时间: 2022
• 期刊: Journal of Chemical Education
• 影响因子: 3
• 作者: Hamilton, Nicholas B.;Remington, Jacob M.;Schneebeli, Severin T.;Li, Jianing
• 通讯作者: Li, Jianing

Chiral Auxiliaries for Stereoselective Electrophilic Aromatic Substitutions

用于立体选择性亲电芳香取代的手性助剂

• DOI: 10.1055/s-0040-1707296
• 发表时间: 2021
• 期刊: Synlett
• 影响因子: 2
• 作者: Sharafi, Mona;Campbell, Joseph P.;Murphy, Kyle E.;Osadchey Brown, Reilly;Schneebeli, Severin T.
• 通讯作者: Schneebeli, Severin T.

Helical Molecular Springs with Varying Spring Constants

具有不同弹簧常数的螺旋分子弹簧

• DOI: 10.1002/anie.202209772
• 发表时间: 2022
• 期刊: Angewandte Chemie International Edition
• 作者: Murphy, Kyle E.;McKay, Kyle T.;Schenkelberg, Mica;Sharafi, Mona;Vestrheim, Olav;Ivancic, Monika;Li, Jianing;Schneebeli, Severin T.
• 通讯作者: Schneebeli, Severin T.