Self-Replicating Catalytic Hybridization Assembly of Bipedal DNAzyme Walkers for Enhanced Electrochemiluminescence Bioanalysis

IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Yan-Mei Lei, Li-Dan Zhao, Ying-Huan Li, Ruo Yuan, Xia Zhong, Ying Zhuo
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引用次数: 0

Abstract

Dynamic DNA nanodevices, particularly DNA walkers, have proven to be versatile tools for target recognition, signal conversion, and amplification in biosensing. However, their ability to detect low-abundance analytes in complex biological samples is often compromised by limited amplification depth and severe signal leakage. To address these challenges, we developed a simple yet highly efficient strategy to engineer a self-replicating bipedal DNAzyme (SEDY) walker for sensitive and selective electrochemiluminescence (ECL) bioanalysis. Unlike conventional DNA walkers that are typically constructed by catalytic DNA assembly in a single direction, the SEDY walker integrates a self-replicating feedback mechanism that greatly enhances both the selectivity and sensitivity of bioanalysis. First, the SEDY walker is assembled through a target-triggered, enzyme-free, self-replicating catalytic approach, minimizing the risk of undesired side reactions and signal leakage by simplifying reactant complexity. Furthermore, the SEDY walker features newly exposed trigger sequences that facilitate its autonomous replication, leading to a robust and exponential amplification of its products. Our experiments demonstrate that the SEDY walker can sensitively and selectively detect acetamiprid by navigating specific probes within cross-shaped DNA orbits. The ECL biosensor offers a linear detection range from 1 × 10–15 M to 1 × 10–9 M, with a limit of detection as low as 5.8 × 10–16 M. We anticipate that the SEDY walker will be a powerful tool for detecting various analytes in biological applications.
用于增强电化学发光生物分析的双足 DNA 酶步行器的自复制催化杂交装配
事实证明,动态 DNA 纳米器件,特别是 DNA 步行器,是生物传感中目标识别、信号转换和放大的多功能工具。然而,它们检测复杂生物样本中低丰度分析物的能力往往因有限的放大深度和严重的信号泄漏而大打折扣。为了应对这些挑战,我们开发了一种简单而高效的策略,设计出一种可自我复制的双足 DNA 酶(SEDY)步行器,用于灵敏而有选择性的电化学发光(ECL)生物分析。与通常通过单向催化 DNA 组装构建的传统 DNA 走行器不同,SEDY 走行器集成了自我复制反馈机制,大大提高了生物分析的选择性和灵敏度。首先,SEDY walker 是通过一种目标触发、无酶、自我复制的催化方法组装而成的,通过简化反应物的复杂性,最大限度地降低了不希望发生的副反应和信号泄漏的风险。此外,SEDY 步进器具有新暴露的触发序列,可促进其自主复制,从而实现其产物的稳健指数扩增。我们的实验证明,SEDY walker 可以在十字形 DNA 轨道内导航特定探针,从而灵敏地、选择性地检测啶虫脒。ECL 生物传感器的线性检测范围从 1 × 10-15 M 到 1 × 10-9 M,检测限低至 5.8 × 10-16 M。
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来源期刊
Analytical Chemistry
Analytical Chemistry 化学-分析化学
CiteScore
12.10
自引率
12.20%
发文量
1949
审稿时长
1.4 months
期刊介绍: Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.
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