基于水滑石空间限域内碳量子点信号放大构建生物体内活性氧化学发光探针

As one of intracellular reactive nitrogen species, peroxynitrite has been implicated as a key pathophysiological intermediate in a growing list of diseases. The detection of peroxynitrite with high sensitivity and high selectivity in living cells still remains a great challenge. In this project, we intend to synthesize carbon dots by taking advantage of the confined space of the two-dimensional interlayer galleries of a layered double hydroxide (LDH) host to limit the in situ growth of carbon dots. On the other hand, we plan to research the mechanisms of the structrue-directed fluorescence performances of LDH-carbon dot hybrid nanocomposites. In addition, As a result, the hole-injected and electron-injected carbon dots were easily formed in the confined space of the two-dimensional interlayer galleries of LDHs by superoxide and hydroxyl radicals, which can be produced from the decomposition of peroxynitrite. Subsequently, the electron-transfer annihilation of hole-injected and electron-injected carbon dots could improve the chemiluminescence (CL) emissions of peroxynitrite. Therefore, we can develop a CL tool to monitor peroxynitrite with high selectivity. This project would open up the new areas of CL behavior in spatial confined space, which have great significances in layered nanomaterial and CL basic theory study and analytical applications.

过氧亚硝酸盐(peroxynitrite, ONOO-)是生物体内一种氮氧活性氧化合物，它在生物体内浓度的变化与一些病理过程息息相关。但由于过氧亚硝酸盐固有的特性对其高灵敏度和高选择性检测具有很大挑战性。本项目拟以水滑石层间限域空间内原位制备碳量子点，并研究水滑石-碳量子点纳米复合材料结构与其荧光信号放大的内在联系。此外，基于过氧亚硝酸盐自身分解产生超氧阴离子自由基和羟自由基，这两种自由基进攻在水滑石限域空间内荧光性能优异的碳量子点通过电子湮灭提高过氧亚硝酸盐的化学发光信号，构筑活细胞内过氧亚硝酸盐专一性化学发光探针。该项目的成功将开辟层状材料空间限域内碳量子点荧光和化学发光行为新领域，对层状纳米材料及活性氧化学发光的基础理论和分析应用研究具有重要意义。

该项目以构筑生物体内活性氧（如过氧亚硝酸盐）发光探针为目标，在水滑石限域空间内原位合成碳量子点，研究生成的水滑石-碳量子点纳米复合材料的荧光和化学发光行为，并利用过氧亚硝酸盐很容易自身分解产生大量羟自由基和超氧阴离子自由基，产生的这两种自由基能进攻水滑石限域空间内碳量子点通过电子湮灭产生更强的化学发光信号，从而实现对生物体内过氧亚硝酸盐专一性化学发光检测。取得如下成果：（1）将水滑石限域效应与化学发光结合起来，开辟了水滑石限域效应表征新方法，深化水滑石结构调控；（2）认识水滑石限域空间调控碳量子点形成的影响机理和规律，对水滑石和碳点制备的基础理论研究具有重要意义；（3）提高化学发光效率，设计高效过氧亚硝酸盐专一性化学发光探针，并拓展到其它活性氧（如羟基自由基）高效化学发光探针。