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基于双适配体功能化磁性硅复合材料的用于检测甲胎蛋白和癌胚抗原的化学发光传感器。

A Chemiluminescence Sensor for the Detection of α-Fetoprotein and Carcinoembryonic Antigen Based on Dual-Aptamer Functionalized Magnetic Silicon Composite.

作者信息

Sun Yuanling, Hou Yanan, Cao Tianzi, Luo Chuannan, Wei Qin

机构信息

Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, PR China.

出版信息

Anal Chem. 2023 May 9;95(18):7387-7395. doi: 10.1021/acs.analchem.3c01056. Epub 2023 Apr 27.

Abstract

In this work, a dual-aptamer functionalized magnetic silicon composite was prepared and used to construct a chemiluminescence (CL) sensor for the detection of α-fetoprotein (AFP) and carcinoembryonic antigen (CEA). First, SiO@FeO was prepared, and polydiallyl dimethylammonium chloride (PDDA) and AuNPs were sequentially loaded on SiO@FeO. Subsequently, the complementary strand of CEA aptamer (cDNA) and the aptamer of AFP (Apt) were attached to AuNPs/PDDA-SiO@FeO. Then, the aptamer of CEA (Apt) and G quadruplex peroxide-mimicking enzyme (G-DNAzyme) were sequentially connected to cDNA, leading to the final composite. Then, the composite was used to construct a CL sensor. When AFP is present, it will combine with Apt on the composite to hinder the catalytic ability of AuNPs to luminol-HO, achieving AFP detection. When CEA is present, it will recognize and bind with Apt, so G-DNAzyme is released to solution and catalyzes the reaction of luminol-HO to achieve CEA determination. After the application of the prepared composite, AFP and CEA were detected in the magnetic medium and supernatant, respectively, after simple magnetic separation. Therefore, the detection of multiple liver cancer markers is realized through the CL technology without additional instruments or technology, which broadens the application range of CL technology. The sensor for detecting AFP and CEA shows wide linear ranges of 1.0 × 10 to 1.0 ng·mL and 0.0001-0.5 ng·mL and low detection limits of 6.7 × 10 ng·mL and 3.2 × 10 ng·mL, respectively. Finally, the sensor was successfully used to detect CEA and AFP in serum samples and provides great potential for detection of multiple liver cancer markers in early clinical diagnosis.

摘要

在本工作中,制备了一种双适配体功能化磁性硅复合材料,并将其用于构建用于检测甲胎蛋白(AFP)和癌胚抗原(CEA)的化学发光(CL)传感器。首先,制备了SiO@FeO,并将聚二烯丙基二甲基氯化铵(PDDA)和金纳米粒子(AuNPs)依次负载在SiO@FeO上。随后,将CEA适配体的互补链(cDNA)和AFP的适配体(Apt)连接到AuNPs/PDDA-SiO@FeO上。然后,将CEA的适配体(Apt)和G-四链体过氧化物模拟酶(G-DNAzyme)依次连接到cDNA上,得到最终的复合材料。接着,将该复合材料用于构建CL传感器。当存在AFP时,它会与复合材料上的Apt结合,阻碍AuNPs对鲁米诺-H₂O₂的催化能力,实现AFP的检测。当存在CEA时,它会识别并与Apt结合,从而使G-DNAzyme释放到溶液中并催化鲁米诺-H₂O₂的反应,实现CEA的测定。在应用制备的复合材料后,经过简单的磁分离,分别在磁性介质和上清液中检测到AFP和CEA。因此,通过CL技术无需额外的仪器或技术即可实现多种肝癌标志物的检测,拓宽了CL技术的应用范围。用于检测AFP和CEA 的传感器显示出宽线性范围,分别为1.0×10⁻⁹至1.0 ng·mL⁻¹和0.0001 - 0.5 ng·mL⁻¹,检测限分别低至6.7×10⁻¹⁰ ng·mL⁻¹和3.2×10⁻¹⁰ ng·mL⁻¹。最后,该传感器成功用于检测血清样本中的CEA和AFP,并为早期临床诊断中多种肝癌标志物的检测提供了巨大潜力。

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