Reversed Isoprenoid Biosynthesis using Isoprene as an Abundant Substrate: A New Pathway to Renewable Hydrocarbon-Based Compounds and Materials

在这个由化学系高分子、超分子和纳米化学项目资助的项目中，阿克伦大学的Judit Puskas将制定策略，量化异戊二烯形成的天然橡胶，并表征形成的聚异戊二烯的微结构。该项目的想法是从根本上了解萜类化合物生物合成中涉及的可逆平衡，并优化异戊二烯的生产，异戊二烯是一种丰富的底物，可以从可再生资源中获得。该方法是使用高分辨率尺寸排除层析、核磁共振光谱以及原位红外和拉曼光谱技术来监测在选定的酶鸡尾酒存在的情况下单体转化的动力学。瓜伊勒和俄罗斯蒲公英的天然橡胶生产也将按照同样的战略进行调查。获得的异戊二烯类化合物的确切结构和摩尔质量将使用各种分析技术来确定，这些数据将用于重建生物合成反应路径。该项目将与法国波尔多大学的Alain Deffieux和西班牙农业基因组研究中心的Manuel Rodriguez-Concepcion合作实施。更广泛的影响包括通过建立多边国际合作来发展研究和教育的基础设施，以及通过该项目及其国际层面促进研究生的教学、培训和学习。该项目将鼓励学生“绿色”思维，找到模仿自然化学途径的方法，并为子孙后代的可持续材料开发做出贡献。异戊二烯和萜类化合物由所有生物产生：植物、微生物和动物。它们在生命过程中具有重要的功能，如呼吸作用、光合作用、生长发育调节等。它们还用于制造重要的弹性材料，这些材料用于一系列行业，如汽车、服装和医疗设备。该项目将有助于更好地了解萜类化合物的生物化学，并导致获得这些化学品的绿色进程。

In this project funded by the Macromolecular, Supramolecular and Nanochemistry Program of the Chemistry Division, Judit Puskas of the University of Akron will develop strategies to quantify the formation of natural rubber, a polyterpenoid, from isoprene and to characterize the microstructure of the polyisoprene formed. The idea of the project is to gain a fundamental understanding of the reversible equilibria involved in terpenoid biosynthesis and to optimize their production from isoprene, an abundant substrate than can be obtained from renewable resources. The approach is to monitor the kinetics of monomer conversion in the presence of selected enzyme cocktails using high resolution size exclusion chromatography, nuclear magnetic resonance spectroscopy, and in situ infrared and Raman spectroscopy techniques. The production of natural rubber from Guayule and Russian Dandelion will also be investigated following the same strategy. The exact structure and molar mass of the obtained isoprenoids will be determined using a variety of analytical techniques, and the data will be used to reconstruct the biosynthetic reaction pathway. The project will be performed in collaboration with Alain Deffieux, University of Bordeaux, France, and Manuel Rodriguez-Concepcion, Centre for Research on Agricultural Genomics (CRAG), Spain. The broader impacts involve developing infrastructure for research and education through establishing multilateral international collaborations as well as promoting teaching, training and learning of graduate students through this project and its international dimensions. The project will encourage students to think "green," finding ways to emulate natural chemical pathways and contributing to sustainable materials development for future generations.Isoprene and terpenoids are produced by all living things: plants, microbes and animals. They have essential functions in life processes such as respiration, photosynthesis, the regulation of growth and development, and others. They are also used to make important elastic materials that are used in a range of industries, such as automotive, apparel, and medical equipment. This project will contribute to a better understanding of the biochemistry of terpenoids and lead to green processes to access these chemicals.