智能水凝胶薄膜电极对生物/药物分子可调控的电催化和电化学传感

The development of effective and convenient method and model for regulation and control of biological/drug molecules in their electrochemical and electrocatalytic behaviors, could provide a feasible method for understanding the catalytic activity and electron transfer mechanism of biological/drug molecules, and is of great significance to the development of new tunable electrochemical biosensor. Smart hydrogel film has become the focus of research because of its good biocompatibility, strong immobilization capacity, plasticity and diversity, as well as changes in the surrounding environment with its unique stimulus-response behavior and performance. By selecting the appropriate constituent, film-forming method and different environmental stimuli, we can regulate and control the permeability of biological/drug or media molecules at the hydrogel film electrodes, and further switch their direct or indirect electrocatalytic behaviors. This project intends to use the combination of stimulus-response hydrogel films (single-layer film of multi-component or layer-by-layer films assembled by different components) and electrocatalysis of biological/drug molecules to regulate and control the physical, the chemical nature of smart hydrogel film, and finally to achieve the purpose of switchable electrocatalysis and electrochemical sensing for biological/drug molecules.

发展有效简便的方法和模型调控生物/药物分子的电化学和电催化行为，可为认识生命体内生物/药物分子的催化活性和电子转移的调控机制提供一种可行的方法，对开发新型的可调控电化学生物传感器具有重要意义。智能水凝胶薄膜因其具有很好的生物相容性、很强的固载能力、可塑性和多样性、以及对周围环境变化具有其独特的刺激响应行为和性能而成为人们研究的焦点。通过选择合适的水凝胶成膜组分、成膜方法和施加不同的环境刺激，可以调控生物/药物或媒介体分子在水凝胶薄膜电极上的通透性，从而进一步调控其直接或间接电催化行为。本项目拟将刺激响应型（多组分单层或层层组装不同单组分）水凝胶薄膜的可调控性与生物/药物分子的电催化相结合，利用调控智能水凝胶薄膜的物理、化学性质来达到调控生物/药物分子的电催化和电化学传感的目的，具有新意。

本项目将刺激响应型水凝胶薄膜的可调控性与生物电催化相结合，利用调控智能水凝胶薄膜的物理、化学性质来达到调控生物电化学催化和电化学传感的目的。通过选择合适的水凝胶成膜组分（N,N-二乙基丙烯酰胺，DEA）、成膜方法（一步自由基聚合的方法）和施加不同的环境刺激（pH、温度和盐浓度），通过调控探针/媒介体分子在水凝胶酶薄膜电极PDEA-GOD-HRP（PDEA：聚N,N-二乙基丙烯酰胺，GOD：葡萄糖氧化酶，HRP：辣根过氧化物酶）、{PAH/PAA}4-(PDEA-HRP) （PAH：聚丙烯胺，PAA：聚丙烯酸）上的通透性，进一步实现了调控水凝胶酶薄膜以铁氰化钾探针分子为媒介体，分别对葡萄糖和过氧化氢的电化学催化氧化、还原。除了主要采用电化学方法外，还采用其他多种方法如红外光谱法与紫外可见、扫描电子显微镜等对水凝胶薄膜进行了表征。通过一系列对比实验探讨了水凝胶酶薄膜对探针通透性的多重开关的机理。在项目执行期的两年中，发表SCI论文1篇，在投SCI论文1篇。培养在读硕士2名、中级职称教师4名。