CAREER: Catalyzing Polymerization in the Laboratory and Discussion in the Classroom with Artificial Metalloenzymes

在这个由化学部化学催化项目资助的项目中，芝加哥大学的Jared C. Lewis教授正在开发由烯烃聚合催化剂组成的人工金属酶（arm），该催化剂与蛋白质支架共价连接，以控制聚烯烃的结构和功能。本研究涉及基于已知烯烃聚合催化剂的辅助因子的合成，不同蛋白质支架的设计和表达，以及利用合成的辅助因子对不同支架进行生物偶联以生成所提出的arm。Argonne国家实验室正在利用光谱学方法和x射线晶体学研究ArM结构的详细特征。研究人员正在探索这些arm催化烯烃聚合的能力，并采用合理设计和定向进化相结合的方法来优化观察到的活性和选择性。鉴于聚烯烃在日常生活中的重要性，该ArM聚合催化剂开发项目正在与Irene C. Hernandez科学促进中学（HMS）的当地中学（8年级）学生一起开发化学、催化和材料教学模块。这将为HMS的学生提供额外的与课程相关的材料化学讨论，并为芝加哥大学的学生提供在现实世界中解释科学并获得教学反馈的机会。这项工作的广泛影响包括发现控制聚合物结构和功能的新机制的潜力，新的功能聚合物，以及化学和蛋白质工程界面的学生和博士后的独特培训机会。本项目主要研究由烯烃聚合催化剂与蛋白质支架共价连接组成的人工金属酶，以控制聚烯烃的结构和功能。研究人员正在探索人工金属酶催化烯烃聚合的能力，并采用合理设计和定向进化相结合的方法来优化观察到的活性和选择性。鉴于聚烯烃在日常生活中的重要性，该催化剂开发项目将与当地中学生一起开发化学、催化和材料方面的教学模块。

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Jared C. Lewis at the University of Chicago is developing artificial metalloenzymes (ArMs) comprised of olefin polymerization catalysts covalently linked to protein scaffolds to control polyolefin structure and function. This research involves the synthesis of cofactors based on known olefin polymerization catalysts, the design and expression of different protein scaffolds, and the bioconjugation of different scaffolds using synthetic cofactors to generate the proposed ArMs. Detailed characterization of ArM structure is being pursued using spectroscopic methods and X-ray crystallography at Argonne National Labs. The ability of these ArMs to catalyze olefin polymerization is being explored, and a combination of rational design and directed evolution is being used to optimize the observed activity and selectivity. Given the importance of polyolefins in every day life, this ArM polymerization catalyst development program is being leveraged to develop teaching modules on chemistry, catalysis, and materials with local middle school (Grade 8) students at the Irene C. Hernandez Middle School for the Advancement of the Sciences (HMS). This will provide HMS students with additional curriculum-relevant discussion of materials chemistry and University of Chicago students with real world opportunities for explaining science and receiving feedback on their teaching. The broader impacts of this work include the potential for discovering new mechanisms to control polymer structure and function, new functional polymers, and unique training opportunities for students and postdocs at the interface of chemistry and protein engineering.This project focuses on the development of artificial metalloenzymes comprised of olefin polymerization catalysts covalently linked to protein scaffolds to control polyolefin structure and function. The ability of artificial metalloenzymes to catalyze olefin polymerization is being explored, and a combination of rational design and directed evolution is being used to optimize the observed activity and selectivity. Given the importance of polyolefins in everyday life, this catalyst development program will be leveraged to develop teaching modules on chemistry, catalysis, and materials with local middle school students.