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

在这项由化学系化学催化计划资助的项目中，芝加哥大学的Jared C.Lewis教授正在开发人工金属酶(ARMS)，该酶由共价连接到蛋白质支架上的烯烃聚合催化剂组成，以控制聚烯烃的结构和功能。这项研究涉及基于已知的烯烃聚合催化剂的辅因子的合成，不同蛋白质支架的设计和表达，以及使用合成的辅因子来产生所建议的手臂的不同支架的生物偶联。阿贡国家实验室正在使用光谱学方法和X射线结晶学对手臂结构进行详细表征。这些臂催化烯烃聚合的能力正在探索中，合理的设计和定向进化的结合正在被用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，艾琳·C·埃尔南德斯科学促进中学(HMS)正在利用这个ARM聚合催化剂开发计划，与当地中学生(8年级)一起开发化学、催化和材料方面的教学模块。这将为HMS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真实世界的机会来解释科学并获得对他们教学的反馈。这项工作的更广泛的影响包括发现控制聚合物结构和功能的新机制的可能性，新的功能聚合物，以及在化学和蛋白质工程领域为学生和博士后提供独特的培训机会。该项目专注于开发由共价连接到蛋白质支架上的烯烃聚合催化剂来控制聚烯烃结构和功能的人造金属酶。人们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，这一催化剂开发计划将被用来开发与当地中学生有关化学、催化和材料的教学模块。

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.