基于相变材料微胶囊的可原位热温调控酶载体的设计构建及其生物催化应用研究

On the basis of a discipline combination of energy conversion & management and biochemical engineering, this proposal will focus on the design and construction of a novel type of thermoregulatory enzyme carrier based on microencapsulated phase change materials (PCMs). Such a type of enzyme carrier exhibits an effective in-situ thermoregulation and good thermal management capabilities to enhance the enzyme activity and storage stability of immobilized enzymes under the fluctuation of ambient temperature. According to the research plan of this proposal, a series of microencapsulated PCMs with different inorganic shells will be first designed and synthesized through self-assembly in a nonaqueous emulsion templating system, and the resultant microcapsules are expected to present the multicomponent, multidimensional and hierarchical structures. The chemical composition, morphology, microstructure, and thermal-storage and thermoregulation performance of the resulting microcapsules will be investigated extensively, and the relationship between their structure and properties will be clarified. The formation mechanisms of hierarchical and multidimensional structures will be carefully explored. Afterward, various enzymes will be immobilized onto the microcapsules as enzyme carriers through covalent bonding, and their immobilization technologies and relevant mechanisms will be investigated intensively. The effects of temperature on the enzyme activity, thermal stability and storage stability of the immobilized enzymes on these carriers will be investigated extensively, and their in-situ thermoregulation mechanism for the enhancement of enzyme activity and biocatalytic efficiency will be studied intensively. Moreover, their separability and reusability will also be investigated. With an enhanced biocatalytic activity, the in-situ thermoregulatory enzyme carriers developed by this proposal will exhibit a great potential for biocatalytic applications and can well serve for sustainable chemistry and green process.

秉承能量转化与管理和生物化工学科交叉与融合的科学理念，提出相变材料微胶囊酶载体的设计思想及其应用研究方案。该酶载体可在工作与储存温度偏离高酶活性温域时，通过芯材相变吸放热来调控其周边微环境温度，使固定化酶处于最佳活性温域，从而增强催化效能。首先运用乳液模板自组装法合成一系列基于不同无机功能壁材并具有多组份、多维度和多层级结构的相变材料微胶囊，重点研究其组成、形貌、微观结构和热温调控功效，探索多维度和多层级结构的构建机制，厘清构效关系，查明合成方法及工艺条件对结构与性能的影响规律。然后重点研究这些酶载体与各种生物酶的固定化技术，查明固定化反应机制；并探索在工作及储存温度显著波动下，酶载体的原位热温调控对增强固定化酶生物活性及储存稳定性的作用功效，揭示其作用机理。利用本项目研究成果，开发出一系列基于相变材料微胶囊的可原位热调控酶载体及相应的酶固定化技术，以满足绿色高效生化工程领域的应用需求。

本课题秉承能量转化与管理和生物化工学科交叉与融合的科学理念，开展了针对基于相变材料微胶囊酶载体的设计、构建及其生物催化应用研究。通过针对不同无机功能壁材并具有多组份、多维度和多层级结构的相变材料微胶囊合成的乳液模板自组装技术研究开发，设计开发了一系列基于介孔SiO2、结晶性TiO2、海胆状CuO、海胆状ZnO、纳米花状MnO2、Ni(OH)2纳米片、和Au纳米粒子、MXene和MOF修饰的多维度表面结构特征的相变材料微胶囊作为可原位热温调控酶载体。通过对上述相变材料微胶囊酶载体的组成、形貌、微观结构和热温调控功效，探索多维度和多层级结构的构建机制研究，厘清了其中的构效关系，查明了合成方法及工艺条件对结构与性能的影响规律。通过对上述相变微胶囊酶载体的热性能研究发现，其可在工作与储存温度偏离高酶活性温域时，通过芯材相变吸放热来调控其周边微环境温度，使固定化酶处于最佳活性温域，从而增强催化效能。重点研究了上述酶载体与各种生物酶的固定化技术，查明了固定化反应机制；通过探索其在工作及储存温度明显波动的情况下，酶载体的原位热温调控对增强固定化酶生物活性及储存稳定性深入研究，发现了微胶囊酶载体的作用功效，揭示了其作用机理。利用本项目研究成果，不仅开发出一系列基于相变材料微胶囊的可原位热调控酶载体及相应的酶固定化技术，用以满足绿色高效生化工程领域的应用需求，还进一步拓展研究，开发出一系列可应用于特异性化合物检测的热温可调控智能生物传感器。研究发现，由相变微胶囊酶载体作为工作电极所构建的电化学生物传感器，在高环境温度下具有比传统生物传感器更高的灵敏度和更低的检测限。从而为开发宽温域使用的智能生物传感器提供了一条崭新的路径。本项目的研究开发为第四代相变材料微胶囊在生物领域中的应用研究开发提供了科学依据和技术支撑。