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制备 V-COF@SWCNTs-COOH/SPCE 负载分子印迹电化学传感器用于实时检测痕量磺胺嘧啶

Preparation of a V-COF@SWCNTs-COOH/SPCE supported molecularly imprinted electrochemical sensor for real-time detection of trace sulfadimidine.

机构信息

Guangdong Provincial Key Laboratory of Food Quality and Safety/ National-Local Joint Engineering Research Center for Precision Machining and Safety of Livestock and Poultry Products, College of Food Science, South China Agricultural University, Guangzhou, 510642, China.

Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang, 515200, China.

出版信息

Talanta. 2025 Jan 1;282:127046. doi: 10.1016/j.talanta.2024.127046. Epub 2024 Oct 15.

Abstract

To overcome the limitations of insufficient sensitivity and poor specificity of portable screen-printed carbon electrode-electrochemical sensors (SPCE-EC) in practical applications, we prepared carrier composites of carboxylic single-walled carbon nanotubes vertically grafted by covalent organic frameworks (v-COF@SWCNTs-COOH) and coated with a molecularly imprinted polymer (MIP) of sulfadimidine (SM). 55 °C hot steam elution is more eco-friendly than traditional organic solvent elution. The results showed that when the mass ratio of DBA to DBA-SWCNTs was 1:1, the v-COF@SWCNTs-COOH obtained by the two-step synthesis method could increase the electrical signal up to 2.33-fold of the bare electrode. The bifunctional monomer MIP prepared on the above structure enhanced the signal response by 2.91-fold, with a high imprint factor of 20. The assembled MIP/v-COF@SWCNTs-COOH/SPCE were analyzed by differential pulse voltammetry (DPV) with a high sensitivity of 0.21 nM for LOD and 0.70 nM for LOQ. In milk and fish samples, the recovery rate was 95.0 %-104.8 %. The validation of authentic pork samples with the statutory LC-MS/MS method showed no significant difference (P > 0.05). The sensor's performance indicators remained robust after five repeated uses. Therefore, the MIP/v-COF@SWCNTs-COOH/SPCE combines the cheapness and portability of SPCE, while the sensitivity and specificity of small molecule detection were significantly improved.

摘要

为了克服便携式丝网印刷碳电极电化学传感器(SPCE-EC)在实际应用中灵敏度不足和特异性差的局限性,我们制备了由共价有机框架(v-COF)垂直接枝的羧酸单壁碳纳米管载体复合材料,并涂覆磺胺嘧啶(SM)的分子印迹聚合物(MIP)。55°C 的热蒸汽洗脱比传统有机溶剂洗脱更环保。结果表明,当两步合成法中 DBA 与 DBA-SWCNTs 的质量比为 1:1 时,所得 v-COF@SWCNTs-COOH 可将裸电极的电信号提高 2.33 倍。在上述结构上制备的双功能单体 MIP 将信号响应提高了 2.91 倍,印迹因子高达 20。组装的 MIP/v-COF@SWCNTs-COOH/SPCE 通过差分脉冲伏安法(DPV)进行分析,LOD 为 0.21 nM,LOQ 为 0.70 nM,具有较高的灵敏度。在牛奶和鱼肉样品中的回收率为 95.0%-104.8%。用法定 LC-MS/MS 方法验证真实猪肉样品,无显著差异(P>0.05)。该传感器在经过五次重复使用后,性能指标仍然保持稳定。因此,MIP/v-COF@SWCNTs-COOH/SPCE 结合了 SPCE 的廉价和便携性,同时显著提高了小分子检测的灵敏度和特异性。

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