Key Laboratory of Theoretical Organic Chemistry and Function Molecule, Ministry of Education Hunan University of Science and Technology, Xiangtan, 411201, Hunan, China.
Hunan Provincial Key Laboratory of Controllable Preparation and Functional Application of Fine Polymers, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan, 411201, Hunan, China.
Anal Bioanal Chem. 2021 Jun;413(15):3847-3859. doi: 10.1007/s00216-021-03355-y. Epub 2021 May 2.
Graphdiyne (GDY) adsorbed DNA probes have been used as a fluorescent sensing platform, but topics including DNA adsorption affinities, DNA probe displacement, and fluorescence quenching ability were rarely researched. Herein, the adsorption affinity of single-stranded DNA (ssDNA) and double-stranded DNA (dsDNA) on a tremella-like GDY was tuned by modulating the surface chemistry of GDY. The fluorescence quenching ability of GDY with different oxidation degrees was compared. The nonspecific displacement of DNA probes on GDY was studied. Under the same concentrations, GDY with low oxidation degree exhibited stronger adsorption affinity and higher adsorption capacity to both ssDNA and dsDNA than highly oxidized GDY. DNA adsorbed on low-oxidized GDY was more resistant to displacement by other DNAs. Protein showed strong interaction with different GDY and could displace DNA probes on GDY. Based on these findings, an ideal GDY with proper oxidation degree, exhibiting high surface affinity for ssDNA and low affinity for dsDNA, was used as scavenger of redundant ssDNA fluorescent probe in an enzyme-assisted amplification system for sensitive ochratoxin (OTA) detection. This study has enhanced our fundamental understanding of DNA adsorption by GDY. It also provided a rational way to apply GDY for fluorescence sensing in a complicated system.
石墨炔（GDY）吸附 DNA 探针已被用作荧光传感平台，但关于 DNA 吸附亲和力、DNA 探针置换和荧光猝灭能力的研究很少。本文通过调节 GDY 的表面化学性质来调整单链 DNA（ssDNA）和双链 DNA（dsDNA）在银耳状 GDY 上的吸附亲和力。比较了不同氧化程度的 GDY 的荧光猝灭能力。研究了 DNA 探针在 GDY 上的非特异性置换。在相同浓度下，低氧化度 GDY 对 ssDNA 和 dsDNA 的吸附亲和力和吸附容量均强于高度氧化的 GDY。吸附在低氧化 GDY 上的 DNA 更能抵抗其他 DNA 的置换。蛋白质与不同的 GDY 表现出强烈的相互作用，能够置换 GDY 上的 DNA 探针。基于这些发现，选择具有适当氧化度的理想 GDY，对 ssDNA 具有高表面亲和力，对 dsDNA 亲和力低，作为酶辅助扩增系统中多余 ssDNA 荧光探针的清除剂，用于灵敏检测赭曲霉毒素（OTA）。本研究增强了我们对 GDY 吸附 DNA 的基本认识。它还为在复杂体系中应用 GDY 进行荧光传感提供了一种合理的方法。
