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Highly Efficient Signal On/Off Electrochemiluminescence Gel Aptasensor Based on a Controlled Release Strategy for the Sensitive Detection of Prostate Specific Antigen
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-03-23 , DOI: 10.1021/acs.analchem.2c05655 Lu Zhao 1 , Xianzhen Song 1 , Dawei Fan 1 , Xuejing Liu 1 , Huan Wang 1 , Qin Wei 1 , Dan Wu 1
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-03-23 , DOI: 10.1021/acs.analchem.2c05655 Lu Zhao 1 , Xianzhen Song 1 , Dawei Fan 1 , Xuejing Liu 1 , Huan Wang 1 , Qin Wei 1 , Dan Wu 1
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The controlled release strategy can make the constructed sensor have the function of self-on/off, which has an obvious effect on improving the sensitivity in immunoassays. Metal organic gels (MOGs) are the most noteworthy. They are materials with ultrahigh surface area, highly dispersed atomical metal sites, and well-defined porosity and can be used as an efficient luminophore to cause the developed sensor to have good hydrophilicity and adjustability, thus further improving the detection sensitivity. In this work, a novel on/off electrochemiluminescence (ECL) gel aptasensor was constructed using the Cys-[Ru(dcbpy)3]2+ gel as a luminophore, ZnS quantum dots (QDs) as quenchers, and aminated mesoporous silica nanocontainers (SiO2–NH2) as carriers of controlled release for prostate specific antigen (PSA) detection. Specifically, the ssDNA and PSA aptamer made up clamp-like molecules to block holes of the SiO2–NH2 after encapsulating the quencher ZnS QDs. Because of the specific binding between the PSA antigen and aptamer, the clamp-like molecules of ssDNA and the PSA aptamer were disassembled. Finally, the release of ZnS QDs was triggered, thereby realizing a self-off mode of the ECL signals under a co-reactant-free environment by ECL resonance energy transfer (ECL-RET) between the Cys-[Ru(dcbpy)3]2+ and ZnS QDs. In addition, the quenching mechanism was confirmed by molecular orbitals from the theoretical calculation level. The detection limit of the gel aptasensor for PSA was as low as 1.01 fg/mL, showing excellent sensitivity and accuracy. These strategies provided a feasible idea for PSA and even other tumor marker immunoassays.
中文翻译：
基于控释策略的高效信号开/关电化学发光凝胶适体传感器用于前列腺特异性抗原的灵敏检测
控释策略可以使构建的传感器具有自开/关功能，对提高免疫测定的灵敏度有明显作用。金属有机凝胶 (MOG) 是最值得注意的。它们是具有超高比表面积、高度分散的原子金属位点和明确孔隙率的材料，可用作高效发光体，使开发的传感器具有良好的亲水性和可调性，从而进一步提高检测灵敏度。在这项工作中，使用 Cys-[Ru(dcbpy) 3 ] 2+凝胶作为发光体、ZnS 量子点 (QD) 作为猝灭剂和胺化介孔二氧化硅纳米容器构建了一种新型开/关电化学发光 (ECL) 凝胶适体传感器( SiO 2 –NH 2) 作为前列腺特异性抗原 (PSA) 检测的控释载体。具体而言，ssDNA 和 PSA 适配体构成钳状分子，以在封装猝灭剂 ZnS QD 后堵塞 SiO 2 –NH 2的孔。由于 PSA 抗原和适体之间的特异性结合，ssDNA 和 PSA 适体的钳状分子被分解。最后，触发 ZnS 量子点的释放，从而通过 Cys-[Ru(dcbpy) 3 ] 之间的 ECL 共振能量转移 (ECL-RET)，实现无共反应环境下 ECL 信号的自关闭模式。2+和 ZnS QD。此外，猝灭机制从理论计算层面得到了分子轨道的证实。PSA 凝胶适体传感器的检测限低至 1.01 fg/mL，显示出出色的灵敏度和准确度。这些策略为 PSA 甚至其他肿瘤标志物免疫检测提供了可行的思路。
更新日期：2023-03-23
中文翻译：
基于控释策略的高效信号开/关电化学发光凝胶适体传感器用于前列腺特异性抗原的灵敏检测
控释策略可以使构建的传感器具有自开/关功能，对提高免疫测定的灵敏度有明显作用。金属有机凝胶 (MOG) 是最值得注意的。它们是具有超高比表面积、高度分散的原子金属位点和明确孔隙率的材料，可用作高效发光体，使开发的传感器具有良好的亲水性和可调性，从而进一步提高检测灵敏度。在这项工作中，使用 Cys-[Ru(dcbpy) 3 ] 2+凝胶作为发光体、ZnS 量子点 (QD) 作为猝灭剂和胺化介孔二氧化硅纳米容器构建了一种新型开/关电化学发光 (ECL) 凝胶适体传感器( SiO 2 –NH 2) 作为前列腺特异性抗原 (PSA) 检测的控释载体。具体而言，ssDNA 和 PSA 适配体构成钳状分子，以在封装猝灭剂 ZnS QD 后堵塞 SiO 2 –NH 2的孔。由于 PSA 抗原和适体之间的特异性结合，ssDNA 和 PSA 适体的钳状分子被分解。最后，触发 ZnS 量子点的释放，从而通过 Cys-[Ru(dcbpy) 3 ] 之间的 ECL 共振能量转移 (ECL-RET)，实现无共反应环境下 ECL 信号的自关闭模式。2+和 ZnS QD。此外，猝灭机制从理论计算层面得到了分子轨道的证实。PSA 凝胶适体传感器的检测限低至 1.01 fg/mL，显示出出色的灵敏度和准确度。这些策略为 PSA 甚至其他肿瘤标志物免疫检测提供了可行的思路。
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