In Situ Self-Assembled Formation of Nitrogen-Rich Ag@Ti3C2 Film for Sensitive Detection and Spatial Imaging of Pesticides with Laser Desorption/Ionization Mass Spectrometry (LDI-MS).
In Situ Self-Assembled Formation of Nitrogen-Rich Ag@Ti3C2 Film for Sensitive Detection and Spatial Imaging of Pesticides with Laser Desorption/Ionization Mass Spectrometry (LDI-MS).
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DOI：
10.1021/acsami.2c22347
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发表时间：
2023-04
影响因子：
9.5
通讯作者：
Wenhan Li;Q. He;Jingchao Li;XiuTeng Zhou;Qiongzheng Hu;Chunxia Ma;Xiao Wang
中科院分区：
文献类型：
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作者：
Wenhan Li;Q. He;Jingchao Li;XiuTeng Zhou;Qiongzheng Hu;Chunxia Ma;Xiao Wang
农药残留危害人体健康；因此，迫切需要开发一种快速灵敏的农药检测方法。本文通过一种生态友好的、紫外线辅助的策略合成了新型富氮Ag@Ti3C2 (Ag@N-Ti3C2)，然后通过简单的水蒸发诱导的自组装过程在目标载体上原位形成了高度均匀的膜。Ag@N-Ti3C2表现出比Ti3C2更大的表面积、导电性和导热性。这种Ag@N-Ti3C2薄膜克服了传统基质的局限性，允许激光解吸/电离质谱（LDI-MS）提供快速和高通量的农药（如多菌灵、噻虫嗪、比威、乐methoate、malathion和氯氰菊酯）分析，具有超高灵敏度（检测限为0.5-200 ng/L）、增强的再现性、极低的本底和良好的耐盐性。农药残留量在0 ~ 4 μg/L范围内呈线性关系（R2 > ~ 0.99）。该Ag@N-Ti3C2薄膜用于中草药和软饮料样品中农药的高通量分析。同时，利用高分辨率Ag@N-Ti3C2薄膜辅助LDI- ms成像技术（LDI MSI），成功探索了植物根系中外源农药及其他内源小分子（如氨基酸、糖类、激素、皂苷等）的空间分布。本研究提出了新的Ag@N-Ti3C2自组装膜均匀沉积在ITO载玻片上，为农药监测提供了双重平台，具有高导电性、准确性、简单性、快速分析、样本量要求最小和成像功能等优点。
Pesticide residues are hazardous to human health; thus, developing a rapid and sensitive method for pesticide detection is an urgent need. Herein, novel nitrogen-rich Ag@Ti3C2 (Ag@N-Ti3C2) was synthesized via an ecofriendly, ultraviolet-assisted strategy, followed by in situ formation of a highly homogeneous film on target carriers via a facile water evaporation-induced self-assembly process. Ag@N-Ti3C2 shows greater surface area, electrical conductivity, and thermal conductivity than Ti3C2. This Ag@N-Ti3C2 film overcomes the limitations of conventional matrixes and allows laser desorption/ionization mass spectrometry (LDI-MS) to provide fast and high-throughput analysis of pesticides (e.g., carbendazim, thiamethoxam, propoxur, dimethoate, malathion, and cypermethrin) with ultrahigh sensitivity (detection limits of 0.5-200 ng/L), enhanced reproducibility, extremely low background, and good salt tolerance. Furthermore, the levels of pesticides were quantified with a linear range of 0-4 μg/L (R2 > 0.99). This Ag@N-Ti3C2 film was used for high-throughput analysis of pesticides spiked in traditional Chinese herbs and soft drink samples. Meanwhile, high-resolution Ag@N-Ti3C2 film-assisted LDI-MS imaging (LDI MSI) was used to successfully explore spatial distributions of xenobiotic pesticides and other endogenous small molecules (e.g., amino acids, saccharides, hormones, and saponin) in the roots of plants. This study presents the new Ag@N-Ti3C2 self-assembled film equably deposits on the ITO slides and provides a dual platform for pesticide monitoring and has the advantages of high conductivity, accuracy, simplicity, rapid analysis, minimal sample volume requirement, and an imaging function.