SGER: Nanoporous Conductive Sol-Gel Biocatalysis for Novel Cofactor Regeneration

摘要提案标题：SGER：用于新型辅因子再生的纳米多孔导电溶胶-凝胶生物催化提案编号：CTS-0538633主要研究者： Chan Beum Park机构： 亚利桑那州立大学分析（决策依据）：该提案将解决氧化还原酶辅因子的关键用途，如昂贵的吡啶辅因子，必须经济地再生用于各种技术应用。 虽然辅因子的电化学再循环已被认为是一种潜在有用的方法，但存在一个明显的障碍，即只有紧邻电极表面的酶才能有效地参与。 这个探索性的研究项目将研究一种高度创新的方法，使用“电子传导”溶胶-凝胶生物反应器进行辅因子再生。 通过在导电溶胶-凝胶混合基质中捕获氧化还原酶并通过操纵纳米多孔凝胶的化学性质，假设辅因子将在整个反应器系统中有效地再循环。 主要研究人员的这种方法显示了对再生过程中关键挑战的敏锐洞察力，但该项目显然具有高风险，因为必须制备用于溶胶-凝胶合成的导电溶胶部分/聚吡咯/石墨/金属颗粒的精确“复合物”，该复合物将基于二氧化硅基溶胶前体，如三烷氧基硅烷。 凝胶前体的化学组成必须与原位辅因子再生效率和所需产物产率的知识仔细相关。 然而，这种方法的成功演示可能会彻底改变生物催化剂电化学再生的适用性。 氧化还原酶辅因子再生的困难和费用是更广泛地合成重要的增值产品（包括药物、食品添加剂、香料、杀虫剂和农药）的关键障碍。 这种方法将开辟一条全新的科学研究途径，并将为基础研究和工程带来新的领域。 在生物传感器和生物燃料电池领域的更广泛的技术应用也是可能的。 研究结果将被纳入上层化学工程课程，这将是一个重大贡献的工程课程的增强。

AbstractProposal Title: SGER: Nanporous Conductive Sol-Gel Biocatalysis for Novel Cofactor RegenerationProposal Number: CTS-0538633Principal Investigator: Chan Beum ParkInstitution: Arizona State UniversityAnalysis (rationale for decision):This proposal will address the critical use of cofactors for oxidoreductases, such as the expensive pyridine cofactor, which must be economically regenerated for a variety of technological applications. Although electrochemical recycling of cofactors has been regarded as a potentially useful approach, there is a clear obstacle in that only enzymes in the immediate vicinity of electrode surface are effectively involved. This exploratory research project will examine a highly innovative approach that uses an "electronically-conductive" sol-gel bioreactor for cofactor regeneration. By entrapping oxidoreductases in a conductive sol-gel hybrid matrix and by manipulating the chemical properties of the nanoporous gel, it is hypothesized that the cofactor will be efficiently recycled throughout the entire reactor system. This approach by the principle investigator shows acute insight into the key challenges in the regeneration process, but the project is clearly high risk because of the necessity of preparing a precise "composite" of conductive sol moiety/polypyrrole/graphite/metal particles for the sol-gel synthesis which would be based on silica-based sol precursors, such as trialkoxysilanes. The chemical composition of the gel precursors must be carefully correlated with knowledge of the in situ cofactor regeneration efficiency and the desired product yield. Successful demonstration of this approach, however, would likely revolutionize the applicability of electrochemical regeneration for biocatalysts. The difficulty and expense of cofactor regeneration for oxidoreductases is a key roadblock for the wider syntheses of important valued-added products including pharmaceuticals, food additives, perfumes, insecticides, and pesticides. This approach would open an entirely new avenue of scientific investigation and would lead to new areas for fundamental research and engineering. Broader technological applications in the areas of biosensors and biofuel cells are also possible. Results from the research will be incorporated into upper-level chemical engineering coursework, which will be a significant contribution to the enhancement of the engineering curriculum.