Harnessing Electroactive Bacteria for Microbial Redox Catalysis

摘要 生物催化剂是合成治疗材料的有力工具，而且 分子。然而，它们通常仅限于进行的天然代谢转化。 通过定义明确的酶。我们假设反应空间服从微生物催化 可通过将来自电活性细菌的呼吸电子通量耦合到氧化还原活性来扩展 过渡金属催化剂在我们称之为微生物氧化还原催化(MRC)的过程中。向我们的 假设并突出了MRC的优势，我们将使用电活性细菌模型 控制与医疗行业相关的几种反应。首先，我们将 拓展和优化多种单体和金属的MRC活性自由基聚合 催化剂。接下来，我们将使用MRC来影响重要药物的脱卤化 先驱物。最后，我们将利用MRC来增强钯催化的交叉偶联 反应。总体而言，我们的计划将结合合成催化剂的机械驱动设计 利用微生物催化剂的可调性为各种健康-提供新的合成路线- 相关的物质和分子。

Abstract Biological catalysts are powerful tools for the synthesis of therapeutic materials and small molecules. Nevertheless, they are typically limited to native metabolic transformations conducted by well-defined enzymes. We hypothesize that the reaction space amenable to microbial catalysis can be extended by coupling respiratory electron flux from electroactive bacteria to redox-active transition metal catalysts in a process we term microbial redox catalysis (MRC). To address our hypothesis and highlight the advantages of MRC, we will use the model electroactive bacterium Shewanella oneidensis to control several reactions relevant to the medical industry. First, we will expand and optimize MRC living radical polymerization for a variety of monomers and metal catalysts. Next, we will use MRC to affect the dehalogenation of important pharmaceutical precursors. Finally, we will leverage MRC to enhance Palladium-catalyzed cross-coupling reactions. Overall, our program will combine the mechanism-driven design of synthetic catalysts with the tunability of microbial catalysts to provide new synthetic routes for a variety of health- relevant materials and molecules.