Polymeric Core-shell Architectures to Adapt Biocatalytically Active Enzymes in Non-aqueous Media with Enhanced Performance

该项目旨在构建聚合物核壳纳米颗粒，其由亲水性内部和疏水性外壳组成，用于封装功能酶，并随后将其转移到具有增强催化性能的有机介质中。为此，一方面，我将逐步建立系统-从建立稳定的聚合物外壳到形成机械强度和生物相容性的核心基质。壳将由合成嵌段共聚物形成，用于形成油包水（w/o）乳液和随后的交联，其中将了解壳稳定性与聚合物性能的相关性。内部核心网络将进一步用生物相容性材料生成，以稳定酶并提高整个基质的机械强度。另一方面，我将在项目的所有阶段使用来自不同的合成重要类别的三种酶，即来自南极假丝酵母的脂肪酶B（CalB）、来自荧光假单胞菌的苯甲醛裂解酶（BAL）和来自近平滑假丝酵母的羰基还原酶（CPCR 2），反复评估和优化系统以增强酶性能（例如酶活性、稳定性和可重复使用性）。通过这种优化，最终将提供一般知识，以通过核-壳平台的聚合物疏水性和微环境生物相容性的定制设计来改善溶剂中的生物催化。此外，该系统将通过不同的显微镜进行物理表征，并通过酶动力学进行定量评估，这可以进一步帮助我们了解载体特性（例如尺寸，溶胀行为和物质沉淀）与催化过程中传质的相关性。作为最终目标，我将应用最佳的核壳胶囊，以证明其在溶剂中的手性化合物的酶促合成的可能性，希望引起更多的兴趣，在该领域的不对称合成领域的封装酶与合理设计的聚合物网络。

The project aims at the construction of polymeric core-shell nanoparticles that consist of a hydrophilic interior and a hydrophobic shell for the encapsulation of functional enzymes as well as subsequent transferring them into organic media with enhanced catalytic performance. For this purpose, on one hand, I will stepwise build up the system - from the establishment of a stable polymer shell to the formation of a mechanically strong and biologically compatible core matrix. The shell will be formed by synthetic block copolymers for the formation of water-in-oil (w/o) emulsions and subsequent cross-linking, where the correlation of shell stability to polymer properties will be learned. The interior core networks will be further generated with biocompatible materials in order to stabilize enzymes and improve the mechanical strength of the whole matrix. On the other hand, I will repeatedly evaluate and optimize the system towards the enhanced enzymatic performance (e.g. enzyme activity, stability, and reusability) using three enzymes from distinct, synthetically important classes, namely lipase B from Candida antarctica (CalB), benzaldehyde lyase from Pseudomonas fluorescens (BAL), and carbonyl reductase from Candida parapsilosis (CPCR2) - at all stages of the project. With such optimization, general knowledge shall be finally provided to improve biocatalysis in solvents by the tailored design of the polymeric hydrophobicity and microenvironmental biocompatibility of core-shell platform. Furthermore, the system will be physically characterized with diverse microscopes and quantitatively assessed by enzyme kinetics, which can further help us get insights into the relevance of carrier properties (e.g. sizes, swelling behavior, and substance precipitation) to the mass transfer during catalysis. As an ultimate goal, I will apply the optimal core-shell capsules to demonstrate its possibility for enzymatic synthesis of chiral compounds in solvents, in hopes to arise more interests in the field of asymmetric synthesis by the encapsulated enzymes with rational design of polymeric networks.