Gold-graphene quantum dot-N-doped porous carbon-based electrochemical aptasensor with DNA amplification for ultrasensitive detection of omethoate

IF 4.9 2区化学 Q1 CHEMISTRY, ANALYTICAL

Microchemical Journal Pub Date : 2025-09-05 DOI:10.1016/j.microc.2025.115181

Dan Xu, Mingyuan Liu, Lizhong Wang, Lei Wang, Hui Yang

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Abstract

The synthesis of highly catalytically active gold‑carbon composites remains a significant challenge. This study reports a novel approach for synthesizing a gold-histidine functionalized graphene quantum dots-N-doped porous carbon composite (Au-HFGQD-NPC). Gold ions (Au³⁺) were coordinated with HFGQD through AuN bonds to form Au-HFGQD complexes, which were then combined with polyacrylamide, freeze-dried, and thermally reduced under a N₂ atmosphere at 500 °C. The resulting Au-HFGQD-NPC features a three-dimensional porous architecture with uniformly dispersed, small Au nanoparticles within the carbon matrix, which enhances its catalytic performance. This composite was utilized as a sensing material to develop an electrochemical aptasensor for omethoate detection that incorporates a DNA recycling amplification strategy. The aptasensor employed a triple-helix aptamer probe (TAP) consisting of an aptamer loop, two segment stems, and a triplex oligonucleotide (probe). Omethoate binding to the aptamer induces the TAP conformational change, releasing the probe. The released probe hybridizes with hairpin DNA 1 (H1) immobilized on the electrode surface via AuS bonds. Subsequently, ferrocene-modified hairpin DNA 2 (H2-Fc) hybridizes with H1, releasing the probe and triggering the next cycle. This recycling mechanism results in the accumulation of multiple H2-Fc molecules on the electrode. The highly catalytically active Au-HFGQD-NPC then catalyzes the oxidation of Fc, leading to a significantly enhanced detection signal. The differential pulse voltammetry peak current exhibited a linear relationship with the logarithm of omethoate concentration over the range of 3 × 10⁻¹⁵ to 1 × 10⁻⁹ M, achieving a detection limit of 1.2 × 10⁻¹⁵ M. The proposed aptasensor demonstrates high sensitivity, selectivity, and stability, and has been successfully applied for determine omethoate in cabbage samples.

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金-石墨烯量子点n掺杂多孔碳基电化学感应传感器的DNA扩增超灵敏检测

高催化活性金碳复合材料的合成仍然是一个重大挑战。本研究报道了一种合成金组氨酸功能化石墨烯量子点- n掺杂多孔碳复合材料（Au-HFGQD-NPC）的新方法。金离子（Au3+）通过AuN键与HFGQD配位形成Au-HFGQD配合物，然后与聚丙烯酰胺结合，在500℃的n2气氛下冷冻干燥，热还原。所得的Au- hfgqd - npc具有三维多孔结构，在碳基体中均匀分散的小Au纳米颗粒增强了其催化性能。该复合材料被用作一种传感材料，用于开发一种包含DNA循环扩增策略的氧化乐果检测的电化学配体传感器。该适体传感器采用三螺旋适体探针（TAP），由适体环、两段茎和三联体寡核苷酸（探针）组成。氧乐果与适体结合诱导TAP构象改变，释放探针。释放的探针通过AuS键与固定在电极表面的发夹DNA 1 （H1）杂交。随后，二茂铁修饰的发夹DNA 2 （H2-Fc）与H1杂交，释放探针并触发下一个周期。这种循环机制导致多个H2-Fc分子在电极上的积累。高催化活性的Au-HFGQD-NPC随后催化Fc氧化，导致检测信号显著增强。差分脉冲伏安法峰电流在3 × 10−15 ~ 1 × 10−9 M范围内与氧乐果浓度的对数呈线性关系，检出限为1.2 × 10−15 M，具有较高的灵敏度、选择性和稳定性，已成功应用于白菜样品中氧乐果的测定。

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来源期刊

Microchemical Journal 化学-分析化学

CiteScore

8.70

自引率

8.30%

发文量

1131

审稿时长

1.9 months

期刊介绍： The Microchemical Journal is a peer reviewed journal devoted to all aspects and phases of analytical chemistry and chemical analysis. The Microchemical Journal publishes articles which are at the forefront of modern analytical chemistry and cover innovations in the techniques to the finest possible limits. This includes fundamental aspects, instrumentation, new developments, innovative and novel methods and applications including environmental and clinical field. Traditional classical analytical methods such as spectrophotometry and titrimetry as well as established instrumentation methods such as flame and graphite furnace atomic absorption spectrometry, gas chromatography, and modified glassy or carbon electrode electrochemical methods will be considered, provided they show significant improvements and novelty compared to the established methods.