2001 TSE: NSF/EPA Novel Self-Assembling Interfacial Biocatalysis in Organic-Aqueous Biphasic Systems for Environmentally Benign Chemical Processing

该项目的目标是功能化水溶性酶，以提供疏水和亲水部分，这是预期的自组装和催化反应在有机-水界面。 将酶置于水溶液或有机溶液中的当前方法对于反应体系而言遭受显著的溶解度和传质限制。 所提出的界面配置为两相系统中的试剂提供了最大限度地接近生物催化剂的途径，从而可以降低溶解度和传质限制。 高分子修饰基团会改变酶分子周围的微环境相互作用，降低界面张力，从而影响酶的界面组装和活化。 与界面组装和反应动力学相关的基本原理，特别是界面张力的影响，将在实验和理论上进行探索。 这种界面生物催化的可行性将被检查和证明的环氧化物和糖苷的酶促生产。 这些酶促合成可能会导致更环保的路线，用于大规模生产有价值的化学品。

The objective of this project is to functionalize water-soluble enzymes to provide hydrophobic and hydrophilic parts, which are expected to self-assemble and catalyze reactions at organic-aqueous interfaces. Current methodologies with enzymes placed in either aqueous or organic solutions suffer significant solubility and mass transfer limitations for reacting systems. The proposed interfacial configuration provides reagents in the biphasic systems the maximum access to the biocatalyst so that solubility and mass transfer limitations can be reduced. The polymeric modifying groups will alter the microenvironmental interactions around the enzyme moieties and reduce the interfacial tension, and thus affect the interfacial assembly and activation of enzymes. Fundamentals related to the interfacial assembly and reaction kinetics, particularly the effect of interfacial tension, will be explored both experimentally and theoretically. The feasibility of this interfacial biocatalysis will be examined and demonstrated for the enzymatic production of epoxides and glycosides. These enzymatic syntheses may lead to more environmentally-friendly routes for large-scale production of valuable chemicals.