Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, China.
Department of Oncology, Division of Life Sciences and Medicine, The First Affiliated Hospital of the University of Science and Technology of China, University of Science and Technology of China, Hefei, Anhui 230001, P.R. China.
Anal Chem. 2023 Aug 29;95(34):12982-12991. doi: 10.1021/acs.analchem.3c03135. Epub 2023 Aug 16.
Recently, magnetic beads (MBs) are moving toward chemiluminescence (CL) functional magnetic nanomaterials with a great potential for constructing label-free immunosensors. However, most of the CL-functionalized MBs suffer from scarce binding sites, easy aggregation, and leakage of CL reagents, which will ultimately affect the analytical performance of immunosensors. Herein, by using core-shell FeO@Au/Ag magnetic nanomaterials as a nanoplatform, a novel -(4-aminobutyl)--ethylisopropanol (ABEI) and Co dual-functionalized magnetic nanomaterial, namely, FeO@Au/Ag/ABEI/Co, with strong and stable CL emission was successfully synthesized. Its CL intensity was 36 and 3.5 times higher than that of MB@ABEI-Au/Co and ABEI and Co dual-functionalized chemiluminescent MBs previously reported by our group, respectively. It was found that the excellent CL performance of FeO@Au/Ag/ABEI/Co could be attributed to the enrichment effect of the Au/Ag shell and the synergistic enhance effect of the Au/Ag shell and Co. A related CL mechanism has been proposed. Afterward, based on the intense and stable CL emission of FeO@Au/Ag/ABEI/Co, a sensitive and effective label-free CL immunosensor for exosome detection was established. It exhibited excellent analytical performance with a wide detection range of 3.1 × 10 to 3.1 × 10 particles/mL and a low detection limit of 2.1 × 10 particles/mL, which were better than the vast majority of the reported CL immunosensors. Moreover, the proposed label-free CL immunosensor was successfully used to detect exosomes in human serum samples and enabled us to distinguish healthy persons and lung cancer patients. It has the potential to be a powerful tool for exosome study and early cancer diagnosis.
最近，磁性珠（MBs）正在向具有构建无标记免疫传感器巨大潜力的化学发光（CL）功能磁性纳米材料发展。然而，大多数 CL 功能化的 MBs 存在结合位点稀少、容易聚集和 CL 试剂泄漏等问题，这最终会影响免疫传感器的分析性能。在此，我们以核壳型 FeO@Au/Ag 磁性纳米材料为纳米平台，成功合成了一种新型 -(4-氨基丁基)-乙基异丙醇（ABEI）和 Co 双功能化磁性纳米材料，即 FeO@Au/Ag/ABEI/Co，其具有强而稳定的 CL 发射。其 CL 强度分别比我们之前报道的 MB@ABEI-Au/Co 和 ABEI 和 Co 双功能化化学发光 MBs 高 36 倍和 3.5 倍。研究发现，FeO@Au/Ag/ABEI/Co 具有优异的 CL 性能，这归因于 Au/Ag 壳的富集效应以及 Au/Ag 壳和 Co 的协同增强效应。提出了相关的 CL 机制。随后，基于 FeO@Au/Ag/ABEI/Co 强而稳定的 CL 发射，建立了一种用于外泌体检测的灵敏有效的无标记 CL 免疫传感器。该传感器具有较宽的检测范围（3.1×10 到 3.1×10 个/mL）和较低的检测限（2.1×10 个/mL），优于绝大多数已报道的 CL 免疫传感器。此外，该无标记 CL 免疫传感器成功地用于检测人血清样本中的外泌体，能够区分健康人和肺癌患者。它有可能成为外泌体研究和早期癌症诊断的有力工具。
