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用于无标记 DNA 阻抗生物传感的修饰石墨烯片。

Decorated graphene sheets for label-free DNA impedance biosensing.

机构信息

Engineering Laboratory for Modern Analytical Techniques, c/o State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, PR China.

出版信息

Biomaterials. 2012 Feb;33(4):1097-106. doi: 10.1016/j.biomaterials.2011.10.045. Epub 2011 Nov 5.

Abstract

An efficient DNA impedance biosensing platform is constructed, in which positively charged N,N-bis-(1-aminopropyl-3-propylimidazol salt)-3,4,9,10-perylene tetracarboxylic acid diimide (PDI) is anchored to graphene sheets. The π-π stacking and electronic interactions are elucidated by the distinct absorption features in UV-vis spectra and by quenching perylene fluorescence in contact with graphene. The rational design and tailoring of graphene surface invest it with desired properties (dispersive, structural, photoelectrical and conductive, etc.) and boost its application. Electrostatic interaction between PDI's positively charged imidazole rings and negatively charged phosphate backbones of single-stranded DNA (ssDNA) facilitates ssDNA immobilization. This manner is different from these mainly based on the attraction between the rings in DNA bases and the hexagonal cells of graphene, which is disturbed after hybridization and causes the leaving of formed double-stranded DNA from graphene surface. The electrostatic ssDNA grafting occupies phosphate backbones and particularly leaves the bases available for efficient hybridization. DNA immobilization and hybridization lead to PDI/graphene interfacial property changes, which are monitored by electrochemical impedance spectroscopy and adopted as the analytical signal. The conserved sequence of the pol gene of human immunodeficiency virus 1 is satisfactorily detected via this PDI/graphene platform and shows high reproducibility, selectivity.

摘要

构建了一种高效的 DNA 阻抗生物传感平台,其中带正电荷的 N,N-双(1-氨丙基-3-丙基咪唑盐)-3,4,9,10-苝四羧酸二酰亚胺(PDI)被锚定在石墨烯片上。通过 UV-vis 光谱中明显的吸收特征以及与石墨烯接触时对苝荧光的猝灭,阐明了 π-π 堆积和电子相互作用。通过合理设计和定制石墨烯表面,赋予其所需的性质(分散性、结构、光电和导电性等),并推动其应用。PDI 的正电荷咪唑环与单链 DNA(ssDNA)的负电荷磷酸骨架之间的静电相互作用促进了 ssDNA 的固定。这种方式与主要基于 DNA 碱基中环与石墨烯六边形单元之间吸引力的方式不同,杂交后这种吸引力会受到干扰,导致形成的双链 DNA 从石墨烯表面离开。静电 ssDNA 接枝占据磷酸骨架,特别是为有效的杂交留出碱基。通过电化学阻抗谱监测 DNA 的固定和杂交引起的 PDI/石墨烯界面性质变化,并将其用作分析信号。通过该 PDI/石墨烯平台可以满意地检测到人免疫缺陷病毒 1 的 pol 基因的保守序列,并表现出高重现性和选择性。

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