Abstract A new method for simultaneously determining cytokeratin fragment antigen 21–1 (CYFRA21-1), carcinoembryonic antigen (CEA), and carbohydrate antigen (CA15–3) was developed using single-particle, ICP-MS-based, magnetic immunoassay. Gold nanoparticles (AuNPs), ZnSe quantum dots (QDs), and Silver nanoparticles (AgNPs) were employed to tag antibodies. A highly efficient capture of CYFRA21-1, CEA, and CA15–3 was achieved using biotinylated, antibody-coated magnetic beads. AuNPs/ZnSe QDs/AgNPs-tagged second antibodies helped realize sensitive quantification of the target antigen using single particle ICP-MS. Under optimum conditions, CYFRA21-1, CEA, and CA15–3 linear concentration ranges were 0.05–50 ng mL−1, 0.02–100 ng mL−1, and 0.6–250 mU mL−1. The correlation coefficients were 0.9999, 0.9987, and 0.9970, respectively. CYFRA21-1, CEA, and CA15–3 detection limits were 0.02 ng mL−1, 0.006 ng mL−1, and 0.25 mU mL−1, respectively. Relative standard deviations (RSD) for CYFRA21-1, CEA, and CA15–3 were 3.2%, 4.4%, and 4.2%, respectively. The method simultaneously detected CYFRA21-1, CEA, and CA15–3 in human lung cancer serum samples with recoveries of between 89.8% and 101%.

中文翻译：

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单粒子ICP-MS结合磁免疫法检测人肺癌血清中三种肿瘤生物标志物

摘要 使用单粒子、基于 ICP-MS 的磁性免疫分析法开发了一种同时测定细胞角蛋白片段抗原 21-1 (CYFRA21-1)、癌胚抗原 (CEA) 和碳水化合物抗原 (CA15-3) 的新方法。金纳米粒子 (AuNPs)、ZnSe 量子点 (QDs) 和银纳米粒子 (AgNPs) 用于标记抗体。使用生物素化、抗体包被的磁珠实现了对 CYFRA21-1、CEA 和 CA15-3 的高效捕获。AuNPs/ZnSe QDs/AgNPs 标记的二抗有助于使用单粒子 ICP-MS 实现目标抗原的灵敏定量。在最佳条件下，CYFRA21-1、CEA 和 CA15-3 的线性浓度范围为 0.05-50 ng mL-1、0.02-100 ng mL-1 和 0.6-250 mU mL-1。相关系数分别为 0.9999、0.9987 和 0.9970。CYFRA21-1, CEA, CA15-3 检测限分别为 0.02 ng mL-1、0.006 ng mL-1 和 0.25 mU mL-1。CYFRA21-1、CEA 和 CA15-3 的相对标准偏差 (RSD) 分别为 3.2%、4.4% 和 4.2%。该方法同时检测了人肺癌血清样品中的 CYFRA21-1、CEA 和 CA15-3，回收率介于 89.8% 和 101% 之间。