Joint Research Center for Precision Medicine, Shanghai Jiao Tong University Affiliated Sixth People's Hospital South Campus, Southern Medical University Affiliated Fengxian Hospital, Shanghai, 201499, China.
School of Chemistry and Chemical Engineering and Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200241, China.
Adv Mater. 2021 Jun;33(24):e2007900. doi: 10.1002/adma.202007900. Epub 2021 May 7.
Self-limited nanoassemblies, such as supraparticles (SPs), can be made from virtually any nanoscale components, but SPs from nanocarbons including graphene quantum dots (GQDs), are hardly known because of the weak van der Waals attraction between them. Here it is shown that highly uniform SPs from GQDs can be successfully assembled when the components are bridged by Tb ions supplementing van der Waals interactions. Furthermore, they can be coassembled with superoxide dismutase, which also has weak attraction to GQDs. Tight structural integration of multilevel components into SPs enables efficient transfer of excitonic energy from GQDs and protein to Tb . This mechanism is activated when Cu is reduced to Cu by nitric oxide (NO)-an important biomarker for viral pulmonary infections and Alzheimer's disease. Due to multipronged fluorescence enhancement, the limit of NO detection improves 200 times reaching 10 × 10 m. Furthermore, the uniform size of SPs enables digitization of the NO detection using the single particle detection format resulting in confident registration of as few as 600 molecules mL . The practicality of the SP-based assay is demonstrated by the successful monitoring of NO in human breath. The biocompatible SPs combining proteins, carbonaceous nanostructures, and ionic components provide a general path for engineering uniquely sensitive assays for noninvasive tracking of infections and other diseases.
自限性纳米组装体，如超粒子（SPs），可以由几乎任何纳米级组件制成，但由于它们之间较弱的范德华吸引力，包括石墨烯量子点（GQDs）在内的纳米碳的 SPs 几乎不为人知。在这里，当组件由补充范德华相互作用的铽离子桥接时，可以成功组装出高度均匀的 GQD SPs。此外，它们可以与超氧化物歧化酶共组装，后者与 GQDs 的吸引力也较弱。多组分的紧密结构集成到 SPs 中，使从 GQDs 和蛋白质到铽的激子能量有效转移。当一氧化氮（NO）将 Cu 还原为 Cu 时，这种机制被激活 - 这是病毒性肺部感染和阿尔茨海默病的重要生物标志物。由于多方面的荧光增强，NO 检测的极限提高了 200 倍，达到 10×10 m。此外，SPs 的均匀尺寸允许使用单个粒子检测格式对 NO 检测进行数字化，从而可以自信地注册少至 600 个分子 mL 。基于 SP 的测定的实用性通过成功监测人类呼吸中的 NO 得到证明。结合蛋白质、碳基纳米结构和离子组件的生物相容性 SPs 为工程提供了一种独特的灵敏测定方法，用于非侵入性跟踪感染和其他疾病。
