高效液相色谱-四极杆飞行时间质谱联用快速分析沉积肽的综合策略:以瓢虫为例。

IF 2.7 2区 化学 Q2 BIOCHEMICAL RESEARCH METHODS
Huijie Sun, Yang Li, Yunhua Feng, Kaicheng Xie, Jinyi Sui, Ting Wu, Hongliang Zhou, Guoliang Dai, Chengyao Ma, Jiandong Zou, Meijuan Xu
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引用次数: 0

摘要

沉积肽是一类结构多样的非核糖体肽,具有广泛的生物活性,由于其复杂的断裂模式,在质谱(MS)中对系统表征提出了重大挑战。本研究旨在建立一种基于高效液相色谱四极杆飞行时间质谱(HPLC-Q-TOF/MS)的通用三步策略,以促进线性和环状沉积肽的快速筛选和鉴定。工作流程由三个顺序的逻辑驱动步骤定义:(1)通过诊断和加合物离子过滤潜在的沉积肽前体以及沉积肽分类;(2)通过监测诊断产物离子和中性损失来识别结构残基;(3)通过MS/MS谱综合分析对多肽主链进行测序。为了验证该策略的通用性,将其应用于复杂生物基质(瓢虫提取物)中沉积肽的分析。总共鉴定或初步表征了62种沉积肽(包括八肽、六肽、四肽和二肽,具有环状和线性拓扑结构),其中包括34种潜在的新型类似物。值得注意的是,该策略成功区分了10种含蛋氨酸的氧化还原修饰的沉积肽(天然蛋氨酸、蛋氨酸亚砜、蛋氨酸砜),证明了其识别结构相似衍生物的能力。这三步策略提供了一个简单,快速,强大的工具,全面的抑郁肽分析。它在复杂基质上的应用突出了扩展到其他生物样品的强大潜力,推进了天然产物和生物系统中沉积肽家族的系统分析。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
An Integrated Strategy for Rapid Profiling of Depsipeptides by High-Performance Liquid Chromatography Coupled to Quadrupole Time-of-Flight Mass Spectrometry: Bombyx batryticatus as an Example.

Depsipeptides, a structurally diverse class of nonribosomal peptides with broad bioactivities, present significant challenges for systematic characterization due to their complex fragmentation patterns in mass spectrometry (MS). This study aims to develop a generic three-step strategy based on high-performance liquid chromatography quadrupole time-of-flight mass spectrometry (HPLC-Q-TOF/MS) to facilitate the rapid screening and identification of both linear and cyclic depsipeptides. The workflow is defined by three sequential, logic-driven steps: (1) filtering potential depsipeptide precursors via diagnostic and adduct ions along with depsipeptide classification; (2) identifying the structural residues by monitoring diagnostic product ions and neutral losses; and (3) sequencing the peptide backbone through comprehensive analysis of MS/MS spectra. To validate the strategy's universality, it was applied to the analysis of depsipeptides in a complex biological matrix (extracts of Bombyx batryticatus). A total of 62 depsipeptides (encompassing octa-, hexa-, tetra-, and didepsipeptides, with both cyclic and linear topologies) were identified or tentatively characterized, including 34 potential novel analogs. Notably, the strategy successfully distinguished 10 methionine-containing depsipeptides with subtle redox modifications (native methionine, methionine sulfoxide, methionine sulfone), demonstrating its ability to resolve structurally similar derivatives. This three-step strategy offers a simple, rapid, and robust tool for comprehensive depsipeptide profiling. Its application to complex matrices highlights the strong potential for extending to other biological samples, advancing systematic analysis of depsipeptide families in natural products and biological systems.

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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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