An Integrative Approach to Metalloenzyme-Catalyzed C-H Activation

该奖项由无机化学、生物无机和金属有机化学项目和国际科学与工程办公室颁发，支持宾夕法尼亚州立大学的Carsten Krebs博士通过动力学、光谱和计算相结合的方法，使用基于几种C-H裂解酶中间体(Fe(IV)-oxo和Fe(III/III)2-Superoxo)的多学科方法来理解C-H激活的基本逻辑。Bollinger/Krebs小组将捕获并表征异青霉素N-合成酶(IPNS)的关键中间体。通过与波恩大学的Frank Neese博士的国际合作，将使用计算方法来阐明电子结构。与宾夕法尼亚州立大学的Hammes-Schiffer小组合作，将使用高级理论来阐明C-H裂解步骤的机制细节。联合的计算研究将成为设计新的实验以检验理论模型的基础。本科生、研究生以及博士后学者将接触到实验化学、生物学和计算化学交界处的跨学科研究。宾夕法尼亚州立大学和波恩大学的研究生和博士后跨境交流和共同咨询将提供独特的培训机会。将为学生和博士后开设生物无机化学暑期工作坊。第二和第四个夏天将在宾夕法尼亚州立大学举办讲习班，第三个夏天将在马克斯·普朗克研究所举办讲习班。这一奖项与波恩大学Frank Neese教授的合作奖项相协调，该奖项由德国联邦基金(DFG)资助。

This award in the Inorganic, Bioinorganic and Organometallic Chemistry program and the Office of International Science and Engineering supports Dr. Carsten Krebs at the Pennsylvania State University to understand the fundamental logic of C-H activation using a multidisciplinary approach based on several C-H-cleaving enzyme intermediates (Fe(IV)-oxo and Fe(III/III)2-superoxo complexes) through a combination of kinetic, spectroscopic and computational methods. The Bollinger/Krebs group will trap and characterize the key intermediates in isopenicllin N-synthase (IPNS). Through an international collaboration with Dr Frank Neese at the University of Bonn computational methods will be used to elucidate the electronic structures. In collaboration with the Hammes-Schiffer group at Penn State, high-level theory will be used to elucidate mechanistic details of the C-H cleavage steps. The combined computational studies will be the basis for the design of new experiments to test the theoretical models. Undergraduate and graduate students, as well as postdoctoral scholars will be exposed to interdisciplinary research at the interface of experimental chemistry and biology and computational chemistry. The exchange and co-advising across borders of graduate students and postdocs from Penn State and the University of Bonn will provide unique training opportunities. Summer workshops in Bioinorganic Chemistry will be developed for students and postdocs. Workshops will be offered at Penn State in the second and fourth summer, and at the Max Planck Institute in the third summer. This award coordinates with a collaborative award to Professor Frank Neese at the University of Bonn funded by the Deutsche Forschungsgemeinschaft (DFG).