富含氨基的硅量子点作为高效活化剂,具有内在化学发光功能,可用于过硫酸盐的检测。

IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Talanta Pub Date : 2025-01-01 Epub Date: 2024-09-22 DOI:10.1016/j.talanta.2024.126931
Dayang Zhao, Hui Gong, Houjing Liu
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引用次数: 0

摘要

由于过硫酸盐(S2O82-,PDS)相关技术的快速发展及其在多个领域的广泛应用,对其进行特异性检测具有重要意义和挑战性。然而,传统的分析方法主要基于其强氧化性,很难同时实现在复杂水环境中特异性识别和高灵敏度检测 PDS。在此,我们特意制备了富含氨基的 SiQDs(N-SiQDs)作为有效催化剂,并引入 H2O2 作为共反应物,以强本征化学发光(CL)来活化和测定 PDS。CL过程中产生了大量活性氧(主要是O2˙-和˙OH),引发了N-SiQDs˙+和N-SiQDs˙-之间的电子-空穴湮灭,从而产生了非凡的CL发射。在此基础上,制备了一种用于检测 PDS 的新型 CL 检测器,其线性范围为 5 × 10-7M-5 × 10-5 M,检测限低(3.2 × 10-7 M)。由于在 CL 发射过程中没有 SO4˙-的参与,该传感平台具有足够的灵敏度和令人满意的选择性,并且不会对过渡金属离子和无机阴离子产生反应,而这些离子在之前报道的 PDS CL 传感器中具有干扰作用。这项工作不仅深化了对纳米材料辅助 PDS 激活机制的认识,而且为改性无金属 QDs CL 探针检测化学物种提供了新的视角。
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Amino-rich silicon quantum dots as efficient activator with intrinsic chemiluminescence for the detection of peroxydisulfate.

The specific detection of peroxydisulfate (S2O82-, PDS) is significant and challenging due to the rapid development of PDS-related technologies and their widespread application in multiple fields. However, traditional analytical methods are mainly based on their strong oxidizing properties, making it difficult to simultaneously achieve specific identification and high sensitivity for PDS detection in complex water environments. Here, we purposely prepared amino-rich SiQDs (N-SiQDs) as an effective catalyst and introduced H2O2 acts as a co-reactant for PDS activation and determination with strong intrinsic chemiluminescence (CL) emission. High yield of reactive active oxygen (mainly O2˙- and ˙OH) were generated during CL process, which trigger electron-hole annihilation between the N-SiQDs˙+ and N-SiQDs˙- accounted for extraordinary CL emission. On this basis, a new CL assay for PDS detection was fabricated with broad linear range of 5 × 10-7M-5 × 10-5 M and low detection limit (3.2 × 10-7 M). Due to the absence of SO4˙- involvement during CL emission, the sensing platform is sensitive enough, satisfactory selectivity and does not respond to transition-metal ions and inorganic anions that have interferences in the PDS CL sensors reported before. This work not only deepens insight into the mechanisms of nanomaterials assisted PDS activation but also provides a new perspective on the modified metal-free QDs CL probe for chemical species detection.

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来源期刊
Talanta
Talanta 化学-分析化学
CiteScore
12.30
自引率
4.90%
发文量
861
审稿时长
29 days
期刊介绍: Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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