具有力学适配性的功能水凝胶膜层材料的设计、制备及其生物电子界面研究

       水凝胶因其与生物体高度相似的特性，如高水含量、离子生理环境和低杨氏模量，成为一种理想的人机交互界面材料。在组织和电极间构筑具有特定功能的水凝胶膜层界面，不仅可以提高二者间的力学适配性，还有助于增强生物电子界面的电交互和物质交换等功能。然而，由于生物体内环境极其复杂，涉及细胞、组织和器官之间的协同相互作用，对水凝胶膜层的功能性和长期稳定性提出了更高的要求。尽管近年来国内外研究学者报道了各类方法提升水凝胶的性能，但当前合成水凝胶依旧存在小分子残留、组织界面的粘合稳定性和可调控性差，以及水凝胶膜层在电极表面的长期稳定性差和功能上无法满足体内特定应用场景需求等挑战，严重制约了水凝胶在生物体内的广泛应用。针对这些挑战，本论文提出了一系列新策略开发功能性水凝胶膜层界面，并对它们的粘附性能、电学性质、生物兼容性、以及在生物体内的实际应用效果进行了深入的研究，旨在通过水凝胶膜层技术推动生物电子领域的快速发展，具体研究内容与结果如下：

     （1）针对合成水凝胶存在的小分子残留及其在生物组织表面粘附稳定性差等挑战，提出了聚合物前驱体的策略，用于开发高生物兼容性的水凝胶粘合剂。在前驱体中分别引入具有生物粘附功能的 N-羟基丁二酰亚胺接枝的聚丙烯酸类高分子，和通过滞后效应起到耗散能量作用的长链聚合物，以及构成三维网络结构的聚合物交联剂；并利用水凝胶干交联方式，可实现水凝胶粘合剂与各种生物组织/工程材料的高韧性粘合，界面韧性高达~150 J m^-2，远高于市售的生物粘合剂（< 20 J m^-2）。良好的生物兼容性和快速韧性组织粘附特性使此类水凝胶粘合剂可用于构筑稳定的组织-器件粘合界面，有助于生理信号的长期高质量记录。

     （2）针对高韧性水凝胶粘合界面可调控性差的挑战，提出了可调控水凝胶粘合界面的设计原则。通过在水凝胶粘合剂体系中引入苯硼酸与二元醇类聚合物的络合作用来提升水凝胶的外在韧性（Γ_D），可实现在湿润的生物组织和工程材料表面的快速高韧性粘合；进一步在生物兼容性刺激下（如喷涂葡萄糖溶液）破坏苯硼酸与二元醇类聚合物的络合作用来降低水凝胶的 Γ_D，可实现韧-脆界面的快速转变，界面韧性由~400 J m^-2下降至~40 J m^-2。使用此类水凝胶粘合剂能够将生物电子牢靠的固定在生物组织表面，并在监测结束后，通过喷洒葡萄糖溶液即可触发生物电子与组织的快速无损分离，不会引发组织损伤等问题。

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