Polarity Gradient Solvent Confinement Membrane Cartridge to Broaden Metabolite Coverage of Plasma Untargeted Analysis

IF 6.7 1区化学 Q1 CHEMISTRY, ANALYTICAL

Analytical Chemistry Pub Date : 2024-11-12 DOI:10.1021/acs.analchem.4c04400

Chunyu Yu, Jiaxin Zhang, Xiaohan Zong, Xiangzi Jin, Lu Liu, Yilin Zou, Yifan Jiao, Meihui Tong, Meiyu Cui, Huwei Liu, Donghao Li

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Abstract

Various polarity chemicals exist in complex samples, such as plasma; nontargeted comprehensive analysis naturally requires multiple polar-extracted solvents; consequently, the polarity of the solvent plays a crucial role in the extraction efficiency of analytes from complex samples. In the present study, based on the diffusion behavior and nanoconfinement effect of solvents in the nanoconfined space, the polarity gradient solvent confinement liquid-phase nanoextraction (PGSC-NLPNE) protocol aimed to perform a one-step nontargeted analysis of a wide range of metabolites in plasma was established. The continuously wide range of extracted solvent polarities on carbon nanofibers/carbon fiber (CNFs/CF) membranes was achieved using a mixture of hexane, dichloromethane, methanol, and water as nanoconfined solvents. The polarities (Log P) of gradient solvents ranged from −1.38 to 3.94. Correlational analyses indicated that metabolites with Log P values ranging from −1.90 to 3.84 were closely related according to similarity-intermiscibility theory. Coupled with a homemade modified guard column device, CNFs/CF membrane cartridge (CCMC), a PGSC-NLPNE-UHPLC-MS online protocol was established and applied in plasma untargeted analysis. By comparing metabolome coverage, reproducibility, and extraction recovery with protein precipitation and two-step liquid–liquid extraction commonly used in untargeted analysis, the PGSC-NLPNE-CCMC protocol demonstrated higher reproducibility and recovery. This protocol has shown great potential for ultrafast analysis of plasma untargeted metabolomics with broader metabolome coverage. It could be a potential tool to rapidly screen out valuable biomarkers related to diseases in the clinic.

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极性梯度溶剂封闭膜盒扩大血浆非靶向分析的代谢物覆盖范围

等离子体等复杂样品中存在多种极性化学物质，非靶向综合分析自然需要多种极性萃取溶剂，因此溶剂的极性对复杂样品中分析物的萃取效率起着至关重要的作用。本研究基于溶剂在纳米约束空间的扩散行为和纳米约束效应，建立了极性梯度溶剂约束液相纳米萃取（PGSC-NLPNE）方案，旨在对血浆中的多种代谢物进行一步法非靶向分析。使用正己烷、二氯甲烷、甲醇和水的混合物作为纳米封闭溶剂，在碳纳米纤维/碳纤维（CNFs/CF）膜上实现了连续宽范围的萃取溶剂极性。梯度溶剂的极性（Log P）范围为-1.38 至 3.94。相关分析表明，根据相似性-互溶性理论，Log P 值在-1.90 至 3.84 之间的代谢物具有密切的相关性。结合自制的改良型保护柱装置--CNFs/CF膜盒（CCMC），建立了PGSC-NLPNE-UHPLC-MS在线分析方案，并将其应用于血浆非靶向分析。通过比较蛋白质沉淀法和两步液液萃取法与非靶向分析中常用的代谢组覆盖率、重现性和萃取回收率，PGSC-NLPNE-CCMC 方案表现出更高的重现性和回收率。该方案在血浆非靶向代谢组学的超快速分析方面显示出巨大潜力，其代谢组覆盖范围更广。它可以作为一种潜在的工具，在临床上快速筛选出与疾病相关的有价值的生物标记物。

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来源期刊

Analytical Chemistry 化学-分析化学

CiteScore

12.10

自引率

12.20%

发文量

1949

审稿时长

1.4 months

期刊介绍： Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.