使用功能化金纳米粒子和卤素键合对新烟碱类农药进行现场检测,ACS Applied Nano Materials

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使用功能化金纳米粒子和卤素键合对新烟碱类农药进行现场检测
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-04-24 , DOI: 10.1021/acsanm.3c00618
Molly M Sherard ₁ , Quang Minh Dang ₁ , Sophia C Reiff ₁ , Jeffrey H Simpson ₁ , Michael C Leopold ₁

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新烟碱类 (NN) 杀虫剂已成为全球使用最广泛的农业工具之一，可保护农作物免受害虫危害并促进粮食生产。不幸的是，一些 NN 化合物，例如广泛使用的基于吡虫啉的杀虫剂，也被确定可能危及蜜蜂等重要的授粉昆虫。为此，NN 农药对世界粮食供应构成潜在威胁。随着越来越多的国家限制或禁止使用 NN 农药，需要工具来有效快速地识别 NN 化合物（如吡虫啉）在现场（例如，在农场的储存区或农药配送仓库）的存在。这项研究代表了一个概念验证，其中能够参与罕见的卤素键合 (XB) 分子间相互作用的特殊改性金纳米粒子 (Au-NP) 的胶体特性可以导致某些 NN 化合物的检测。密度泛函理论和扩散有序核磁共振光谱 (DOSY NMR) 用于探索强 XB-供体结构与 NN 化合物之间的基本 XB 相互作用，发现后者具有多个 XB-受体结合位点。对这些 XB 相互作用的基本理解允许对链烷硫醇盐稳定的 Au-NPs 进行功能化，称为单层保护金簇 (MPC)，具有 XB 供体能力（密度泛函理论和扩散有序核磁共振光谱 (DOSY NMR) 用于探索强 XB-供体结构与 NN 化合物之间的基本 XB 相互作用，发现后者具有多个 XB-受体结合位点。对这些 XB 相互作用的基本理解允许对链烷硫醇盐稳定的 Au-NPs 进行功能化，称为单层保护金簇 (MPC)，具有 XB 供体能力（密度泛函理论和扩散有序核磁共振光谱 (DOSY NMR) 用于探索强 XB-供体结构与 NN 化合物之间的基本 XB 相互作用，发现后者具有多个 XB-受体结合位点。对这些 XB 相互作用的基本理解允许对链烷硫醇盐稳定的 Au-NPs 进行功能化，称为单层保护金簇 (MPC)，具有 XB 供体能力（f -MPC）。在某些 NN 化合物（如吡虫啉）存在的情况下，f -MPC 随后表现出 XB 诱导的可见聚集，该聚集也用吸收（UV-vis）光谱测量并用透射电子显微镜（TEM）成像验证。展示的f -MPC 聚集检测方案具有许多有利的属性，包括快速报告 NN 目标的存在，仅需要微克的可疑物质，以及对吡虫啉（最普遍和最重要的 NN 杀虫剂化合物）具有高度选择性。不需要仪器，所提出的方法可以被设想为一个简单的筛选测试，其中将未知粉末的棉签从表面浸入f-MPC 解决方案导致f -MPC 聚集并产生吡虫啉存在的初步迹象。

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On-Site Detection of Neonicotinoid Pesticides Using Functionalized Gold Nanoparticles and Halogen Bonding

Neonicotinoid (NN) pesticides have emerged globally as one of the most widely used agricultural tools for protecting crops from pest damage and boosting food production. Unfortunately, some NN compounds, such as extensively employed imidacloprid-based pesticides, have also been identified as likely endangering critical pollinating insects like honey bees. To this end, NN pesticides pose a potential threat to world food supplies. As more countries restrict or prohibit the use of NN pesticides, tools are needed to effectively and quickly identify the presence of NN compounds like imidacloprid on site (e.g., in storage areas on farms or pesticide distribution warehouses). This study represents a proof-of-concept where the colloidal properties of specifically modified gold nanoparticles (Au-NPs) able to engage in the rare intermolecular interaction of halogen bonding (XB) can result in the detection of certain NN compounds. Density functional theory and diffusion-ordered NMR spectroscopy (DOSY NMR) are used to explore the fundamental XB interactions between strong XB-donor structures and NN compounds, with the latter found to possess multiple XB-acceptor binding sites. A fundamental understanding of these XB interactions allows for the functionalization of alkanethiolate-stabilized Au-NPs, known as monolayer-protected gold clusters (MPCs), with XB-donor capability (f-MPCs). In the presence of certain NN compounds such as imidacloprid, the f-MPCs subsequently exhibit visual XB-induced aggregation that is also measured with absorption (UV–vis) spectroscopy and verified with transmission electron microscopy (TEM) imaging. The demonstrated f-MPC-aggregation detection scheme has a number of favorable attributes, including quickly reporting the presence of the NN target, requiring only micrograms of suspect material, and being highly selective for imidacloprid, the most prevalent and most important NN insecticide compound. Requiring no instrumentation, the presented methodology can be envisioned as a simple screening test in which dipping a cotton swab of an unknown powder from a surface in a f-MPC solution causes f-MPCs to aggregate and yield a preliminary indication of imidacloprid presence.

更新日期：2023-04-24

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