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基于双功能DNA链介导的从金@银纳米立方体到银纳米簇的转变对细菌脂多糖进行表面增强拉曼散射和电化学发光双模式传感

SERS and ECL dual-mode sensing of bacterial lipopolysaccharide based on bifunctional DNA strands mediated transformation from Au@Ag nanocubes to silver nanoclusters.

作者信息

Sun Yudie, Feng Aobo, Zhang Ruilai, Quan Kehong, Hua Zefeng, Zhang Kui

机构信息

School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma Xiang Road, Ma 'anshan, Anhui 243032, PR China; Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, Qingdao University of Science and Technology, Qingdao 266042, PR China.

School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma Xiang Road, Ma 'anshan, Anhui 243032, PR China.

出版信息

J Hazard Mater. 2025 May 5;488:137283. doi: 10.1016/j.jhazmat.2025.137283. Epub 2025 Jan 18.

Abstract

Bacterial contamination is a very serious health and environmental problem, with the main source of toxicity being lipopolysaccharides in the cell walls of Gram-negative bacteria. Therefore, the development of effective analytical methods is crucial for the detection of lipopolysaccharide content. This work facilitates the efficient generation of precisely adjustable dual-mode signals for LPS detection in surface-enhanced Raman spectroscopy (SERS) and electrochemiluminescence (ECL) by inducing anisotropic morphological evolution of Au@Ag nanocubes (Au@AgNCs) through poly-cytosine (poly-C) DNA. In the presence of LPS, the released probe triggers rolling circle amplification (RCA) and generates cyclic poly-C DNA, which subsequently induces the etching of Ag composites on Au@AgNCs. This etching process leads to changes in both the morphology and composition of Au@AgNCs composite materials, resulting in a decrease in SERS signals. The poly-C DNA was subsequently adsorbed with Ag and then reduced to silver nanoclusters (AgNC) by NaBH, serving as an ECL signal source. Under optimal experimental conditions, both SERS and ECL demonstrated linear ranges spanning from 1 fg/mL to 1 ng/mL, with detection limits of 0.29 fg/mL and 0.14 fg/mL, respectively. Moreover, the SERS-ECL dual-mode sensor facilitates the accurate discrimination of Gram-negative bacteria in diverse real samples. It demonstrates promising applications in the areas of food safety, water quality monitoring, and clinical bacterial detection.

摘要

细菌污染是一个非常严重的健康和环境问题,毒性的主要来源是革兰氏阴性菌细胞壁中的脂多糖。因此,开发有效的分析方法对于检测脂多糖含量至关重要。这项工作通过聚胞嘧啶(poly-C)DNA诱导Au@Ag纳米立方体(Au@AgNCs)的各向异性形态演变,促进了表面增强拉曼光谱(SERS)和电化学发光(ECL)中用于脂多糖检测的精确可调双模式信号的高效生成。在脂多糖存在的情况下,释放的探针触发滚环扩增(RCA)并生成环状聚胞嘧啶DNA,随后诱导Au@AgNCs上的银复合材料蚀刻。这种蚀刻过程导致Au@AgNCs复合材料的形态和组成发生变化,导致SERS信号降低。随后,聚胞嘧啶DNA吸附银,然后通过硼氢化钠还原为银纳米团簇(AgNC),作为电化学发光信号源。在最佳实验条件下,SERS和ECL的线性范围均为1 fg/mL至1 ng/mL,检测限分别为0.29 fg/mL和0.14 fg/mL。此外,SERS-ECL双模式传感器有助于准确区分各种实际样品中的革兰氏阴性菌。它在食品安全、水质监测和临床细菌检测等领域显示出广阔的应用前景。

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