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Ratiometric Fluorescence Detection of DNA Based on the Inner Filter Effect of Ru(bpy)₂(dppx)²⁺ toward Silicon Nanodots.

ABSTRACT: A ratiometric DNA sensor was developed based on fluorescent silicon nanodots (SiNDs) and Ru(bpy)₂(dppx)²⁺. The absorption spectrum of Ru(bpy)₂(dppx)²⁺ has significant overlap with both the excitation and emission spectra of SiNDs. Therefore, fluorescence quenching of Ru(bpy)₂(dppx)²⁺ toward SiNDs can occur on account of the strong inner filter effect. The effect of quenching is not influenced by the specific binding between Ru(bpy)₂(dppx)²⁺ and DNA. Fluorescence turn-on detection of DNA can be performed employing Ru(bpy)₂(dppx)²⁺ and SiNDs as the response and reference signals, respectively. Using SiND-Ru(bpy)₂(dppx)²⁺, a convenient, sensitive, rapid, and precise method could be developed for DNA detection. In aqueous solutions, the I ₆₀₁/I ₄₄₈ fluorescence intensity ratio of SiND-Ru(bpy)₂(dppx)²⁺ increases linearly in the DNA concentration range of 20-1500 nM. The limit of detection and precision of the method is 4.3 nM and 3.5% (50 nM, n = 13), respectively. The ratiometric sensor was tested for visual detection of trace DNA. Moreover, this method was found suitable for the ratiometric detection of DNA in a simulated sample and a human serum sample, and the recoveries were in the range of 98-119%.

SUBMITTER: Zhang Y

PROVIDER: S-EPMC7808131 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Publications

Ratiometric Fluorescence Detection of DNA Based on the Inner Filter Effect of Ru(bpy)2(dppx)2+ toward Silicon Nanodots.

Zhang Yanan Y Hou Dajun D Zhao Bingshan B Li Chunyin C Wang Xiaoyan X Xu Lanying L Long Tao T

ACS omega 20201231 1

A ratiometric DNA sensor was developed based on fluorescent silicon nanodots (SiNDs) and Ru(bpy)2(dppx)2+. The absorption spectrum of Ru(bpy)2(dppx)2+ has significant overlap with both the excitation and emission spectra of SiNDs. Therefore, fluorescence quenching of Ru(bpy)2(dppx)2+ toward SiNDs can occur on account of the strong inner filter effect. The effect of quenching is not influenced by the specific binding between Ru(bpy ...[more]

PMID: 33458536

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Project description:Photochemical CO2 reduction catalysed by trans(Cl)-Ru(bpy)(CO)2Cl2 (bpy = 2,2'-bipyridine) efficiently produces carbon monoxide (CO) and formate (HCOO-) in N,N-dimethylacetamide (DMA)/water containing [Ru(bpy)3]2+ as a photosensitizer and 1-benzyl-1,4-dihydronicotinamide (BNAH) as an electron donor. We have unexpectedly found catalyst concentration dependence of the product ratio (CO/HCOO-) in the photochemical CO2 reduction: the ratio of CO/HCOO- decreases with increasing catalyst concentration. The result has led us to propose a new mechanism in which HCOO- is selectively produced by the formation of a Ru(i)-Ru(i) dimer as the catalyst intermediate. This reaction mechanism predicts that the Ru-Ru bond dissociates in the reaction of the dimer with CO2, and that the insufficient electron supply to the catalyst results in the dominant formation of HCOO-. The proposed mechanism is supported by the result that the time-course profiles of CO and HCOO- in the photochemical CO2 reduction catalysed by [Ru(bpy)(CO)2Cl]2 (0.05 mM) are very similar to those of the reduction catalysed by trans(Cl)-Ru(bpy)(CO)2Cl2 (0.10 mM), and that HCOO- formation becomes dominant under low-intensity light. The kinetic analyses based on the proposed mechanism could excellently reproduce the unusual catalyst concentration effect on the product ratio. The catalyst concentration effect observed in the photochemical CO2 reduction using [Ru(4dmbpy)3]2+ (4dmbpy = 4,4'-dimethyl-2,2'-bipyridine) instead of [Ru(bpy)3]2+ as the photosensitizer is also explained with the kinetic analyses, reflecting the smaller quenching rate constant of excited [Ru(4dmbpy)3]2+ by BNAH than that of excited [Ru(bpy)3]2+. We have further synthesized trans(Cl)-Ru(6Mes-bpy)(CO)2Cl2 (6Mes-bpy = 6,6'-dimesityl-2,2'-bipyridine), which bears bulky substituents at the 6,6'-positions in the 2,2'-bipyridyl ligand, so that the ruthenium complex cannot form the dimer due to the steric hindrance. We have found that this ruthenium complex selectively produces CO, which strongly supports the catalytic mechanism proposed in this work.

Dataset Information

Ratiometric Fluorescence Detection of DNA Based on the Inner Filter Effect of Ru(bpy)₂(dppx)²⁺ toward Silicon Nanodots.

Publications

Ratiometric Fluorescence Detection of DNA Based on the Inner Filter Effect of Ru(bpy)<sub>2</sub>(dppx)<sup>2+</sup> toward Silicon Nanodots.

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