China Light Industry Key Laboratory of Meat Microbial Control and Utilization, School of Food and Biological Engineering, Hefei University of Technology, Hefei 230009, China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230027, China.
ACS Appl Mater Interfaces. 2023 Mar 8;15(9):12570-12579. doi: 10.1021/acsami.2c22607. Epub 2023 Feb 21.
Toward the challenge on reliable determination of trace fentanyl to avoid opioid overdose death in drug crisis, here we realize rapid and direct detection of trace fentanyl in real human urine without pretreatment by a portable surface enhanced Raman spectroscopy (SERS) strategy on liquid/liquid interfacial (LLI) plasmonic arrays. It was observed that fentanyl could interact with the gold nanoparticles (GNPs) surface, facilitate the LLI self-assembly, and consequently amplify the detection sensitivity with a limit of detection (LOD) as low as 1 ng/mL in aqueous solution and 50 ng/mL spiked in urine. Furthermore, we achieve multiplex blind sample recognition and classification of ultratrace fentanyl doped in other illegal drugs, which has extremely low LODs at mass concentrations of 0.02% (2 ng in 10 μg of heroin), 0.02% (2 ng in 10 μg of ketamine), and 0.1% (10 ng in 10 μg of morphine). A logic circuit of the AND gate was constructed for automatic recognition of illegal drugs with or without fentanyl doping. The data-driven analog soft independent modeling model could quickly distinguish fentanyl-doped samples from illegal drugs with 100% specificity. Molecular dynamics (MD) simulation elucidates the underlying molecular mechanism of nanoarray-molecule co-assembly through strong π-metal interactions and the differences in the SERS signal of various drug molecules. It paves a rapid identification, quantification, and classification strategy for trace fentanyl analysis, indicating broad application prospects in response to the opioid epidemic crisis.
为了应对可靠测定痕量芬太尼以避免毒品危机中阿片类药物过量死亡的挑战，我们在此实现了无需预处理即可在液体/液体界面（LLI）等离子体阵列上通过便携式表面增强拉曼光谱（SERS）策略快速且直接检测真实人体尿液中的痕量芬太尼。我们观察到芬太尼可以与金纳米粒子（GNPs）表面相互作用，促进 LLI 自组装，从而将检测灵敏度提高到在水溶液中的检测限（LOD）低至 1 ng/mL，在尿液中加标的检测限（LOD）低至 50 ng/mL。此外，我们实现了超痕量芬太尼掺杂在其他非法药物中的盲样识别和分类，其质量浓度的 LOD 非常低，在海洛因中为 0.02%（10 μg 中 2 ng），在氯胺酮中为 0.02%（10 μg 中 2 ng），在吗啡中为 0.1%（10 μg 中 10 ng）。构建了与门的逻辑电路，用于自动识别是否掺杂芬太尼的非法药物。基于数据驱动的模拟软独立建模模型可以快速区分掺杂芬太尼的样品和不含芬太尼的非法药物，特异性为 100%。分子动力学（MD）模拟通过强π-金属相互作用和不同药物分子的 SERS 信号的差异阐明了纳米阵列-分子共组装的潜在分子机制。它为痕量芬太尼分析提供了快速识别、定量和分类策略，表明在应对阿片类药物流行危机方面具有广阔的应用前景。
