Simultaneous multiplexed quantification of caffeine and its major metabolites theobromine and paraxanthine using surface-enhanced Raman scattering.
Simultaneous multiplexed quantification of caffeine and its major metabolites theobromine and paraxanthine using surface-enhanced Raman scattering.
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DOI：
10.1007/s00216-015-9004-8
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发表时间：
2015-11
影响因子：
4.3
通讯作者：
Goodacre R
中科院分区：
文献类型：
--
作者：
Alharbi O;Xu Y;Goodacre R
对药物及其代谢物进行准确的定量测量很重要，因为这可以用来确定非法材料的长期滥用情况，以及为合法疗法确定准确的药物剂量。然而，在人体体液中发现的药物和异物代谢物的水平需要高度敏感的方法，以及可重复性和便携性的潜力。拉曼光谱确实提供了极好的重复性、便携性和化学特异性，但不幸的是，除非增强，否则拉曼效应通常太弱。因此，我们发展了表面增强拉曼散射(SERS)，并将其与人工神经网络强大的机器学习技术相结合，实现了对咖啡因及其两种主要代谢物可可碱和对黄嘌呤的快速定量。我们建立了从10−5到10−7 Mol/dm 3的三向混合分析，并对三种分析物在三级混合物中的预测都很好。我们选择的范围反映了人体体液中的水平，我们的便携式表面增强拉曼光谱分析的典型误差是咖啡因为1.7 × 10−6 /dm~3，可可碱为8.8 ×−10 /dm~3，对黄嘌呤为9.6 × 10−7 mm o l/dm~3。我们相信，这展示了使用SERS同时对多个分析物进行定量分析的令人兴奋的前景，而不需要求助于冗长而耗时的层析，而这种方法通常必须与质谱学相结合。本文的在线版本(doi：10.1007/s002160159004-8)包含补充材料，授权用户可以使用。
Accurate quantitative measurement of drugs and their metabolites is important as this can be used to establish long-term abuse of illicit materials as well as establish accurate drug dosing for legal therapeutics. However, the levels of drugs and xenometabolites found in human body fluids necessitate methods that are highly sensitive as well as reproducible with the potential for portability. Raman spectroscopy does offer excellent reproducibility, portability and chemical specificity, but unfortunately, the Raman effect is generally too weak unless it is enhanced. We therefore developed surface-enhanced Raman scattering (SERS) and combined it with the powerful machine learning technique of artificial neural networks to enable rapid quantification of caffeine and its two major metabolites theobromine and paraxanthine. We established a three-way mixture analysis from 10−5 to 10−7 mol/dm3, and excellent predictions were generated for all three analytes in tertiary mixtures. The range we selected reflects the levels found in human body fluids, and the typical errors for our portable SERS analysis were 1.7 × 10−6 mol/dm3 for caffeine, 8.8 × 10−7 mol/dm3 for theobromine and 9.6 × 10−7 mol/dm3 for paraxanthine. We believe this demonstrates the exciting prospect of using SERS for the quantitative analysis of multiple analytes simultaneously without recourse to lengthy and time-consuming chromatography, a method that often has to be combined with mass spectrometry. The online version of this article (doi:10.1007/s00216-015-9004-8) contains supplementary material, which is available to authorized users.