生物质谱

质谱已成为生物和生物化学研究的一个重要的分析工具,特别是在蛋白质组学研究的作用更显突出.它的分析速度、准确性和灵敏度都是传统分析技术所不可比拟的.主要介绍了两种近年来发展最为迅速、应用最为广泛的软离子化质谱技术:即基体辅助激光解吸离子化质谱(MALDI-MS)和电喷雾离子化质谱(ESI-MS)的原理、技术的最新进展,并简单介绍了它们在蛋白质和多肽分析中的应用.     

常压敞开式离子化质谱技术研究进展

近年来,无需复杂样品前处理、且在开放环境下实现离子化的常压敞开式离子化质谱技术( Ambientionization mass spectrometry,AI - MS)的研制与应用成为质谱学领域的前沿及备受关注的研究方向.该文综述了AI离子源的基本原理、特征与应用进展,并结合笔者研制的空气动力辅助离子化(Air flow assisted ionization,AFAI)技术,介绍了气流辅助常压敞开式离子化技术的基本特点及其应用.展望了常压敞开式离子化技术的发展趋势.     

基于等离子体原理的新型有机质谱离子化技术

近年来,等离子体在有机化合物解吸与离子化中的作用日益凸显,基于等离子体的各类有机质谱离子化新技术不断涌现.该类技术在灵敏度、分析速度上较传统的离子化方法有大幅度提升,使得它们在复杂样品原位分析中具有显著优势.本综述重点介绍等离子体离子化技术在近3年的最新进展,评述它们与本课题组近期开发的火焰离子化、碳纤维离子化技术在原理、装置及应用方面的异同和相互联系,并探讨这类技术的发展趋势.     

复杂样品质谱分析技术的原理与应用

原位、实时、在线、非破坏、高通量、低耗损的质谱学方法是质谱分析技术发展的重要趋势.在无需样品预处理的条件下对复杂基体样品中痕量待测物直接离子化技术的出现,极大地提高了质谱分析的效率,使实际样品的快速质谱分析成为可能.本文着重综述了能够在无需样品预处理情况下对复杂基体样品离子化的新兴质谱技术及其应用研究,系统阐述了直接离子化技术的基本原理和方法,介绍了几种典型的常压直接离子化技术和装置,对直接离子化质谱分析技术在食品、药品、环境、活体分析、代谢组学、蛋白质组学以及生物组织质谱成像等领域的典型应用进行了述评,讨论了提高复杂样品快速质谱分析选择性的可能方法,并展望了常压直接离子化技术未来发展的可能趋势.     

敞开式离子化质谱在贸易产品化学风险物质筛查中的应用及前景

敞开式离子化质谱是一种新兴的质谱快检技术,具有分析速度快、操作流程简单、特异性强等特点.该技术无需对样品做复杂预处理,尤其在与便携式质谱仪联用时,可用于大量样品的现场、快速、准确筛查,在贸易产品化学风险物质的筛查中展现出广泛的应用前景.该文主要综述敞开式离子化质谱近年来在贸易产品化学风险物质筛查方面的研究进展,并对其未...     

实时直接分析质谱新技术及其应用

由于不需要复杂的样品前处理过程,并具有实时、原位分析等特点,常压敞开式离子化技术成为近年来质谱研究的热点之一.实时直接分析(direct analysis in real time,DART)是近年来出现的一种常压敞开式离子化新技术,在食品安全、环境监测、爆炸物检测以及生物医药等诸多研究领域均有广泛的应用.本文简单介绍了常压敞开式离子化方法的发展,DART的基本原理和研究现状.进而介绍了我国质谱研究人员在基于DART的质谱仪器改进、联用技术以及生物药物等检测分析方面取得的新进展和新成果.     

质谱常压离子化技术的新进展

质谱法是一种重要的分析方法,被广泛应用于生物工程、化学、材料科学、生命科学、医学、环境监测等领域。质谱技术一个多世纪来的巨大发展与离子化技术的进步紧密相关,离子化源被认为是质谱仪的心脏。本文对近年来在常压离子化技术方面的新进展进行了评述。     

引言

质谱技术兼具灵敏度高、选择性强、分析速度快等优势,是现代分析测试领域的"金标准".质谱聚焦于离子的产生、操控、分离和测量,离子化技术的突破革新推动了质谱技术的跨越发展.近年来,无需复杂样品前处理、可在常压环境下实现直接样品分析的敞开式电离质谱技术成为质谱分析领域备受关注的研究热点.自解吸电喷雾电离和实时直接分析问世以来...     

等离子体常压解吸离子源质谱

近年来,常压开源质谱解吸/离子化(ambient desorption/ionization mass spectrometry)技术的开发促进了质谱分析的蓬勃发展.作为常压开源质谱技术的一大重要分支,基于等离子体的常压质谱解吸/离子化技术因无需样品预处理、无溶剂化过程、高灵敏度、高通量、能实时在线检测样品等优点,受到了学术界及仪器制造、化学和生物分析等相关产业界的广泛关注.本文从离子源的种类、原理及应用等角度对目前我国在开源质谱领域中自主研发的基于等离子体的常压离子源的研究进展进行了总结,并对此类等离子体常压离子源的发展进行了展望,重点涉及微波等离子体源、常压微辉光放电等离子体源和解吸电晕束离子源.     

单细胞质谱分析方法研究进展

细胞的个体差异性对于生物体生理功能的运行至关重要,准确阐释相关生物学机理需要以单细胞化学组分的准确测量为基础。然而,由于单细胞中的物质含量低、组成复杂,且不同物质的含量差异大,导致单细胞分析的技术难度极大。质谱技术凭借其高灵敏度、高特异性,以及强大的结构解析能力,近年来在单细胞分析研究中得到了广泛应用。研究者已建立了多种质谱分析方法,实现了单细胞中不同物质的准确测量。从离子化技术的角度,单细胞质谱分析方法目前主要包括三类,即纳升电喷雾离子化质谱法、激光解吸附离子化质谱法和二次离子质谱法。本文对近年基于上述三种离子化技术的单细胞质谱分析方法的研究进展进行了归纳和总结,对单细胞质谱分析方法未来的发展趋势进行了展望。     

Air flow assisted ionization for remote sampling of ambient mass spectrometry and its application

Ambient ionization methods are an important research area in mass spectrometry (MS) analysis. Under ambient conditions, the gas flow and atmospheric pressure significantly affect the transfer and focusing of ions. The design and implementation of air flow assisted ionization (AFAI) as a novel and effective, remote sampling method for ambient mass spectrometry are described herein. AFAI benefits from a high extracting air flow rate. A systematic investigation of the extracting air flow in the AFAI system has been carried out, and it has been demonstrated not only that it plays a role in the effective capture and remote transport of charged droplets, but also that it promotes desolvation and ion formation, and even prevents ion fragmentation during the ionization process. Moreover, the sensitivity of remote sampling ambient MS analysis was improved significantly by the AFAI method. Highly polar and nonpolar molecules, including dyes, pharmaceutical samples, explosives, drugs of abuse, protein and volatile compounds, have been successfully analyzed using AFAI-MS. The successful application of the technique to residue detection on fingers, large object analysis and remote monitoring in real time indicates its potential for the analysis of a variety of samples, especially large objects. The ability to couple this technique with most commercially available MS instruments with an API interface further enhances its broad applicability.     

嗜酸性氧化亚铁硫杆菌代谢产物的常压化学电离质谱分析

本研究以721矿和745矿嗜酸性氧化亚铁硫杆菌为研究对象,采用常压化学电离质谱直接分析其代谢产物,分别考察了顶空采样( Headspace sampling)、界面采样( Interface sampling)和中性解吸采样( Neutral desorption sampling)3种进样方式对电离效果的影响。在优化条件下,常压化学电离质谱对微生物纯菌种和混合菌种的代谢产物均具有良好的分析能力,可根据获得的代谢产物指纹谱图结合主成分分析( PCA)方法和聚类分析( CA)方法区分2个放射性强弱不同区域共4类嗜酸性微生物样品,并对主要胺类、酯类等代谢成分进行串联质谱鉴定,为耐辐射微生物的相关研究提供了一种可借鉴的分析方法。     

敞开式电离质谱技术在法医毒物分析中的应用

敞开式电离质谱(Ambient ionization mass spectrometry,AIMS)是指在大气压环境下,无需或只需简单的样品前处理即可对样品中目标物进行分析的质谱技术.AIMS具有简单、快速、无损和适用范围广等优势,被广泛应用于法医毒物分析领域.该文对敞开式电离(Ambient ionization,A...     

Ambient mass spectrometry: bringing MS into the “real world”

Mass spectrometry has recently undergone a second contemporary revolution with the introduction of a new group of desorption/ionization (DI) techniques known collectively as ambient mass spectrometry. Performed in an open atmosphere directly on samples in their natural environments or matrices, or by using auxiliary surfaces, ambient mass spectrometry (MS) has greatly simplified and increased the speed of MS analysis. Since its debut in 2004 there has been explosive growth in the applications and variants of ambient MS, and a very comprehensive set of techniques based on different desorption and ionization mechanisms is now available. Most types of molecules with a large range of masses and polarities can be ionized with great ease and simplicity with the outstanding combination of the speed, selectivity, and sensitivity of MS detection. This review describes and compares the basis of ionization and the concepts of the most promising ambient MS techniques known to date and illustrates, via typical analytical and bioanalytical applications, how ambient MS is helping to bring MS analysis deeper than ever into the “real world” open atmosphere environment—to wherever MS is needed.     

Desorption sonic spray ionization for (high) voltage-free ambient mass spectrometry

Sonic spray ionization is shown to create a supersonic cloud of charged droplets able to promote efficient desorption and ionization of drugs directly from the surfaces of commercial drug tablets at ambient conditions. Compared with desorption electrospray ionization (DESI), desorption sonic spray ionization (DeSSI) is advantageous since it uses neither heating nor high voltages at the spray capillary. DeSSI therefore provides a more friendly environment in which to perform ambient mass spectrometry (MS). DeSSI-MS is herein evaluated for the analysis of drug tablets, and found to be, in general, as sensitive as DESI-MS. The (high) voltage-free DeSSI method provides, however, cleaner mass spectra with less abundant solvent cluster ions and with enough abundant analyte signal for tandem mass spectrometry (MS/MS). These features may therefore facilitate the DeSSI-MS detection of low molar mass components or impurities, or both. The higher-velocity supersonic DeSSI spray also facilitates matrix penetration thus providing more homogenous sampling and longer lasting ion signals.     

Data-Independent Microbial Metabolomics with Ambient Ionization Mass Spectrometry

Atmospheric ionization methods are ideally suited for prolonged MS/MS analysis. Data-independent MS/MS is a complementary technique for analysis of biological samples as compared to data-dependent analysis. Here, we pair data-independent MS/MS with the ambient ionization method nanospray desorption electrospray ionization (nanoDESI) for untargeted analysis of bacterial metabolites. Proof-of-principle data and analysis are illustrated by sampling Bacillus subtilis and Pseudomonas aeruginosa directly from Petri dishes. We found that this technique enables facile comparisons between strains via MS and MS/MS plots which can be translated to chemically informative molecular maps through MS/MS networking. The development of novel techniques to characterize microbial metabolites allows rapid and efficient analysis of metabolic exchange factors. This is motivated by our desire to develop novel techniques to explore the role of interspecies interactions in the environment, health, and disease. This is a contribution to honor Professor Catherine C. Fenselau in receiving the prestigious ASMS Award for a Distinguished Contribution in Mass Spectrometry for her pioneering work on microbial mass spectrometry.

原位电离与小型质谱在公共安全领域的应用

质谱作为一种具有高准确度、高灵敏度、高选择性的检测仪器,在公共安全领域有着重要的应用前景.公共安全领域的需求主要涉及毒品、毒物、爆炸物等化学物质的现场快速检测,因其影响广泛,检测结果需非常准确.作为实验室分析仪器,质谱的准确性和速度能满足公共安全的应用需求,但作为现场快速检测的仪器仍需要一定改进.现场快速检测一方面要求...     

真空紫外光电离质谱技术进展及其在快速分析中的应用

真空紫外光电离源(VUV-PI)是一种普适性的质谱软电离源,真空紫外光电离质谱谱图无碎片、易解析、灵敏度高,适合于在线快速分析.真空紫外光电离质谱根据分析对象不同可以直接采用单光子电离或添加掺杂剂实现化学电离,能实现气、液、固体分析,也可实现成像分析.该文介绍了真空紫外光电离源的电离原理、光源类型,分析了光电离质谱灵敏...     

电喷雾电离质谱在化学中应用新进展

电喷雾电离质谱(ESI-MS)是本世纪发展的非常重要的质谱,具有无碎片的特点,可分析检测非挥发性的、极性的、热不稳定的化合物。评述了ESI-MS在富勒烯化学、无机配合物、簇合物、有机化学反应,金属有机化合物及超分子化学中的应用进展。