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利用组装在黑磷纳米片上的聚黄尿酸对循环肿瘤DNA进行自信号电化学识别。

Self-signal electrochemical identification of circulating tumor DNA employing poly-xanthurenic acid assembled on black phosphorus nanosheets.

作者信息

Yan Xinyu, Zhang Wei, Yang Jimin

机构信息

School of Chemistry and Chemical Engineering, Linyi University, Linyi, 276000, China.

School of Chemistry and Chemical Engineering, Linyi University, Linyi, 276000, China.

出版信息

Anal Biochem. 2024 Jul;690:115512. doi: 10.1016/j.ab.2024.115512. Epub 2024 Mar 26.

DOI:10.1016/j.ab.2024.115512
PMID:38527608
Abstract

A self-signal electrochemical identification interface was prepared for the determination of circulating tumor DNA (ctDNA) in peripheral blood based on poly-xanthurenic acid (PXTA) assembled on black phosphorus nanosheets (BPNSs) acquired through simple ultrasonication method. The BPNSs with large surface area could be integrated with the xanthurenic acid (XTA) monomers by right of physisorption, and hence improved the electropolymerization efficiency and was beneficial to the enlargement of the signal response of PXTA. The assembled PXTA/BPNSs composite with attractive electrochemical activity was adopted as a platform for the recognition of DNA immobilization and hybridization. The probe ssDNA was covalently fixed onto the PXTA/BPNSs composite with plentiful carboxyl groups through the terminate free amines of DNA probes by use of the 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide and N-hydrosulfosuccinimide cross-linking reaction, accompanied with the decline of the self-signal response. When the hybridization between the probe ssDNA and the target DNA was accomplished, the self-signal response of the composite interface reproduced by virtue of the shaping of helix construction. The determination limit of the assembled DNA identification interface was 2.1 × 10 mol/L, and the complementary target DNA concentrations varied from 1.0 × 10 mol/L to 1.0 × 10 mol/L. The DNA identification platform displayed magnificent sensitivity, specificity and stability, and was efficaciously implemented to the mensuration of ctDNA derived from colorectal cancer.

摘要

基于通过简单超声法制备的组装在黑磷纳米片(BPNSs)上的聚黄尿酸(PXTA),制备了一种自信号电化学识别界面,用于测定外周血中的循环肿瘤DNA(ctDNA)。具有大表面积的BPNSs可通过物理吸附与黄尿酸(XTA)单体结合,从而提高电聚合效率,有利于扩大PXTA的信号响应。将具有诱人电化学活性的组装PXTA/BPNSs复合材料用作DNA固定和杂交识别的平台。通过1-乙基-3-(3-二甲基氨基丙基)碳二亚胺和N-氢磺基琥珀酰亚胺交联反应,利用DNA探针的末端游离胺将探针单链DNA共价固定在具有大量羧基的PXTA/BPNSs复合材料上,同时伴随着自信号响应的下降。当探针单链DNA与靶DNA完成杂交时,由于螺旋结构的形成,复合界面的自信号响应得以恢复。组装的DNA识别界面的测定限为2.1×10 mol/L,互补靶DNA浓度在1.0×10 mol/L至1.0×10 mol/L之间变化。该DNA识别平台表现出出色的灵敏度、特异性和稳定性,并有效地应用于结直肠癌来源的ctDNA的测定。

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