新型合成阿片类药物的互补分离。

IF 2.7 2区 化学 Q2 BIOCHEMICAL RESEARCH METHODS
Andrew R. Forero, , , Samuel A. Miller, , , Lilian Valadares Tose, , , Matthew Willetts, , , Mark E. Ridgeway, , , Melvin A. Park, , , Elisa N. Shoff, , and , Francisco Fernandez-Lima*, 
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引用次数: 0

摘要

芬太尼类似物的日益流行和多样性引起了国际社会的直接关注。在美国,芬太尼及其类似物是致死性和非致死性过量用药的主要原因。最近与芬太尼有关的过量用药事件归因于芬太尼的非法生产,其特点是其特别强效。在这项研究中,我们提出了一种基于高通量质谱的芬太尼类似物有效筛选方法,重点是利用商业上可用的平台,结合液相色谱法、捕获离子迁移率谱法和串联质谱法(LC-TIMS-q-TOF MS/MS)进行同分异构体分离。基于同位素模式、保留时间、迁移谱和质谱模式,该分析方法可以有效地分离和鉴定250种合成阿片类药物。我们的方法利用了在液相色谱时间尺度上使用碰撞诱导解离的迁移陷阱中平行积累随后的顺序碎片(PASEF)的进步。虽然单个同分异构体类似物通常观察到单个色谱带,但大多数芬太尼类似物通常观察到归因于两个质子化位点的双迁移谱带。参考迁移率由高分辨率(RIMS≈80-120)采集的0.2% RSD的单一标准品报告。增加的迁移率分离导致了同分异构体化合物的分离而不影响LC-q-TOF MS/MS分析的灵敏度;也就是说,所有合成类似物具有良好的线性动态和(R2 > 0.98),低检出限(LOD)在0.08-4 ng/mL范围内(LOD < 1 ng/mL可观察到~ 100个类似物)。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Complementary Separation of Novel Synthetic Opioids

Complementary Separation of Novel Synthetic Opioids

The escalating prevalence and diversity of fentanyl analogues poses an immediate concern for the global community. Fentanyl and its analogues are the primary contributors to both fatal and nonfatal overdoses in the United States. The most recent instances of fentanyl-related overdoses have been attributed to the illicit production of fentanyl, characterized by its exceptionally potent nature. In this study, we present a high-throughput mass spectrometry based method for effective screening of fentanyl analogues with focus on the isomeric separation using commercially available platforms combining liquid chromatography, trapped ion mobility spectrometry, and tandem mass spectrometry (LC-TIMS-q-TOF MS/MS). The proposed analysis allows for effective separation and identification of 250 synthetic opioids based on the isotopic pattern, retention time, mobility profile, and MS/MS pattern. Our approach capitalizes on the advancements incorporating parallel accumulation in the mobility trap followed by sequential fragmentation (PASEF) using collision-induced dissociation on the liquid chromatography time scale. While a single chromatography band is commonly observed for single isomeric analogues, a dual mobility band profile attributed to two protonation sites is commonly observed for most fentanyl analogues. Reference mobility values are reported from single standards with 0.2% RSD collected at high resolution (RIMS ≈ 80–120). The added mobility separation resulted in the separation of isomeric compounds without compromising the sensitivity of the LC-q-TOF MS/MS analysis; that is, a good linear dynamic and (R2 > 0.98) and low limits of detection (LOD) in the 0.08–4 ng/mL range were observed for all synthetic analogues (∼100 analogues can be observed with LOD < 1 ng/mL).

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来源期刊
CiteScore
5.50
自引率
9.40%
发文量
257
审稿时长
1 months
期刊介绍: The Journal of the American Society for Mass Spectrometry presents research papers covering all aspects of mass spectrometry, incorporating coverage of fields of scientific inquiry in which mass spectrometry can play a role. Comprehensive in scope, the journal publishes papers on both fundamentals and applications of mass spectrometry. Fundamental subjects include instrumentation principles, design, and demonstration, structures and chemical properties of gas-phase ions, studies of thermodynamic properties, ion spectroscopy, chemical kinetics, mechanisms of ionization, theories of ion fragmentation, cluster ions, and potential energy surfaces. In addition to full papers, the journal offers Communications, Application Notes, and Accounts and Perspectives
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