多形态DNA调控的银纳米团簇荧光特性和细胞成像研究-生物工程专业论文.docxVIP

ABSTRACT Fluorescent metal nanoclusters (FMNCs) are molecular aggregate containing from several to dozens of noble metal atoms. As a novel class of fluorescent materials, FMNCs have unique optical and photophysical properties, which are used in analytes detection and celluar imaging. Particularly, DNA-templated silver nanoclusters (Ag NCs), with the advantages of facile synthesis, tunable fluorescence emission, and good biocompatibility, have attracted increasing interests in biosensing and bionanotechnology. However, it is so far elusive yet what the relationships are between the structural composition of DNA sequences and the fluorescent properties of Ag NCs. The preparation Ag NCs with desirable properties through designing suitable DNA templates have became a hot topic in the scientific community. In this article, interactions of Ag+ with polymorphic DNA templates involving G-quadruplex, i-motif, C-rich strand, and duplex were investigated through ITC. The formation of different DNA-Ag+ complexes is a strongly enthalpy driven process. The binding ratio for the duplex is the highest, and the binding ratio for G-quadruplex is much samller. The binding affinities of Ag+ greatly depend on the secondary structures of DNA templates, with a decreasing order: C-rich strand i-motif duplex G-quadruplex. Fluorescent Ag NCs prepared using these DNA templates possess the emission wavelength from 538 nm to 706 nm. Among them, [C4A4C3]-Ag exhibit the highest fluorescent quantum yield of 37%. Their fluorescence stabilities are associated with the binding affinities between DNA templates and Ag+, e.g., C4A4C3 with the highest binding constant (40.2×105 M?1) stabilizes Ag NCs for over 300 h, while G4T4G4 with the lowest binding constant (0.64×105 M?1) generates Ag NCs with the shortest shelf-life (50 h). In addition, HeLa cells were successfully labeled by using Lipofectamine as a transfection agent to incorporate the red emitting [C4A4C3]-Ag and the NIR emitting [G4T4G4-