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使用自电化学发光氧化石墨烯封端的 Au@L012 纳米复合材料检测阿托摩尔抗原。

Attomole Antigen Detection Using Self-Electrochemiluminous Graphene Oxide-Capped Au@L012 Nanocomposite.

机构信息

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University , Nanjing 210093, China.

出版信息

Anal Chem. 2017 Feb 21;89(4):2418-2423. doi: 10.1021/acs.analchem.6b04305. Epub 2017 Feb 9.

Abstract

In this work, a self-electrochemiluminous graphene oxide-capped Au@L012 nanocomposite was prepared as the label at carcinoembryonic (CEA) antibody to detect attomole CEA antigen. To maximize the luminescence intensity, L012 molecules (luminol analogue) were linked with poly(diallyldimethylammonium chloride) (PDDA) to form positive charged PDDA&L012 pairs, which were modified on negative charged Au@nafion nanoparticles to construct a Au@nafion@PDDA&L012 (Au@L012) complex. Graphene oxide with carboxyl groups was capped at Au@L012 complex through electrostatic interaction to serve as an effective matrix for the covalent attachment of CEA antibody. As compared with the traditional used Au nanoparticles modified with luminol, ∼740-fold increase of self-luminescence was observed from this new complex so that CEA antigen as low as 0.5 amol at electrode surface was measurable in the absence of any coreactant. Moreover, the nanocomposite was attached with CEA antigen at MCF-7 cells allowing the detection of CEA antigen from 72 cells. The success in the detection of surface antigen at small population of cells suggested the self-electrochemiluminescence nanocomposite as the new and biosafe label for the ECL immunoassay, which might push the application of ECL for the cellular immunoanalysis.

摘要

在这项工作中,制备了一种自电化学发光氧化石墨烯封端的 Au@L012 纳米复合材料,作为癌胚抗原(CEA)抗体的标记物,用于检测皮摩尔级的 CEA 抗原。为了最大限度地提高发光强度,将 L012 分子(鲁米诺类似物)与聚二烯丙基二甲基氯化铵(PDDA)连接,形成带正电荷的 PDDA&L012 对,然后将其修饰在带负电荷的 Au@nafion 纳米粒子上,构建 Au@nafion@PDDA&L012(Au@L012)复合物。带羧基的氧化石墨烯通过静电相互作用封端在 Au@L012 复合物上,作为 CEA 抗体共价连接的有效基质。与传统的用鲁米诺修饰的 Au 纳米粒子相比,该新复合物的自发光强度提高了约 740 倍,因此在没有任何辅助反应物的情况下,电极表面的 CEA 抗原低至 0.5 皮摩尔即可检测到。此外,该纳米复合材料与 MCF-7 细胞上的 CEA 抗原结合,允许从 72 个细胞中检测到 CEA 抗原。成功地在小群体细胞表面抗原的检测表明,自电化学发光纳米复合材料是用于 ECL 免疫分析的新型生物安全标记物,这可能推动 ECL 在细胞免疫分析中的应用。

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