An Integrative Approach to Metalloenzyme-Catalyzed C-H Activation

金属酶催化 C-H 活化的综合方法

• 批准号: 0724084
• 负责人: Carsten Krebs
• 金额: $ 36.6万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2007
• 资助国家: 美国
• 起止时间: 2007-08-15 至 2010-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0724084&HistoricalAwards=false
• 关键词: Integrative; Approach; Metalloenzyme; Catalyzed; Activation

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).

这个无机、生物无机和有机金属化学项目和国际科学与工程办公室的奖项支持宾夕法尼亚州立大学的Carsten Krebs博士通过动力学、光谱和计算方法的结合，使用基于几种碳氢切割酶中间体(Fe（IV)-氧和Fe(III/III)2-超氧络合物）的多学科方法来理解碳氢活化的基本逻辑。Bollinger/Krebs小组将捕获和表征异霉素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，计算方法将用于阐明电子结构。在与宾夕法尼亚州立大学哈默斯-希弗小组的合作中，高层次的理论将用于阐明碳氢裂解步骤的机械细节。联合计算研究将成为设计新实验以检验理论模型的基础。本科生和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联合指导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研讨会，第三个夏天将在马克斯普朗克研究所举办研讨会。该奖项与德国研究协会（DFG）资助的波恩大学Frank Neese教授的合作奖相协调。