基于有机−无机纳米复合水凝胶的活性氧化学发光成像研究

Reactive oxygen species (ROS) present some characteristics that make their imaging analysis still an enormous challenge, namely their very short lifetime and high reactivity. Chemiluminescence (CL) imaging analysis has drawn consistent attention of researchers by virtue of its background-free signal and high sensitivity. Among various ROS-related CL system, luminol-based systems provide obvious advantages in bioanalytical applications due to their high luminescence quantum yield and water solubility. However, the CL duration of luminol-based systems is relatively short, which significantly restricting their applications in CL imaging. In this project, we intend to synthesize organic‒inorganic nanocomposite hydrogels with excellent CL performance. Intense and long-lasting CL signals from luminol‒hydrogen peroxide system can be obtained through combining the space confinement from the three-dimensional micro-/nano- network structure of hydrogels and the surface confinement from the two-dimensional rigid layer of layered double hydroxides. The mechanism of the CL time-extension under the synergistic confinement will be investigated in depth. Taking the most common ROS hydrogen peroxide for research object, a novel CL imaging platform can be constructed for the ROS analysis in vivo. The implementation of this project will expand the application of organic‒inorganic nanocomposites in CL analysis, and provide new strategies for the CL imaging analysis of ROS.

活性氧因其寿命短、活性高等特点，在生物体内的成像分析仍然极具挑战。化学发光成像分析以其无背景干扰、灵敏度高等优点，引起了学者们的广泛关注。在活性氧相关的化学发光体系中，鲁米诺体系以其较高的发光量子产率和水溶性的特点，在生物分析中展现出明显的优势。但其发光时间较短，极大地限制了其在化学发光成像分析中的应用。本项目拟结合水凝胶三维微/纳米网孔结构的空间限域和水滑石二维刚性层板的表面限域效应，制备化学发光性能优异的有机−无机纳米复合水凝胶，同时实现鲁米诺−过氧化氢体系化学发光的增强和延时，探寻并揭示协同限域微环境下延时化学发光行为的本质。以最常见的活性氧过氧化氢为研究对象，构建生物体内活性氧化学发光成像分析新平台。本项目的开展将拓展有机−无机纳米复合材料在化学发光分析中的应用，为实现活性氧的化学发光成像分析提供新的思路。

细胞内的活性氧水平变化对于揭示相关疾病的致病机理、开发药物等具有重要意义。活性氧因其寿命短、活性高等特点，在生物体内的高选择性、高灵敏检测仍然极具挑战。本项目利用纳米材料的空间限域及表面限域效应，开发了化学发光性能优良的有机-无机纳米复合材料，构建了水相适用的活性氧化学发光检测体系，成功构筑了过氧化氢和次氯酸根的高灵敏化学发光探针，并验证了其用于细胞内活性氧检测的可行性。本项目的开展将拓展有机-无机纳米复合材料在化学发光分析中的应用，为构筑高灵敏度、高特异性的活性氧化学发光探针提供了新思路，对活性氧相关的疾病诊断治疗和生理病理学研究和具有一定的理论价值和实际应用价值。