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院士致辞
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The rapid and quantitative analysis of anthropogenic contaminants in environmental matrices is crucial for regulatory testing and to elucidate the environmental fate of these pollutants. Direct ambient mass spectrometry (AMS) methodologies greatly increase sample throughput, can be adapted for onsite analysis and are often regarded as semi-quantitative by most developed protocols. One of the limitations of AMS, especially for on site analysis applications, is the irreproducibility of the measurements related to the occurrence of transient microenvironments (TME) and variable background interferences. In this work we report an effective strategy to minimize these effects by hyphenating, for the first time, solid phase microextraction (SPME) arrow to mass spectrometry via a thermal desorption unit (TDU) and direct analysis in real time (DART) source. The developed method was optimized for the extraction and analysis of pesticides and pharmaceuticals from surface water. It was demonstrated that the hyphenation of the SPME and TDU-DART resulted in reduced background contamination, indicating the suitability of the method for onsite analysis even in variable and non-ideal environments. Model analytes were quantitated in the low μg/L range with a total analysis time of less than 5 min, linear dynamic ranges (LDR) and interday reproducibility for most compounds being 2.5–500 μg/L and lower than 10%, respectively. The developed approach provides an excellent analytical tool that can be applied for the onsite high-throughput analysis of water samples as well as air and aereosols. Considering the tunability of our extraction process, time-resolved environmental monitoring can be achieved onsite within minutes.
环境基质中人为污染物的快速定量分析对于监管检测至关重要。原位质谱(AIMS)极大地提高了样品通量,适用于现场分析。对于现场分析应用,瞬态微环境(TME)和可变背景可能干扰重现性。在这项工作中,我们开发了一种有效的策略,将固相微萃取(SPME)与质谱联用,通过热解吸单元(TDU)和实时直接分析离子源(DART)来最小化这些影响。该方法适用于地表水中杀虫剂和药物的提取和分析。结果表明,SPME 和 TDU-DART 联用降低了背景污染,即使在可变和非理想环境中也能够进行现场分析。模型分析物在低浓度范围内定量,总分析时间小于5分钟,大多数化合物的线性动态范围(LDR)和日间现性分别为2.5-500μg/L和低于10%。该方法提供了一种优异的分析工具,用于水样以及空气和土壤的现场高通量分析,并且可在几分钟内实现现场环境监测。
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包膜病毒是一个重要的公共卫生问题,其中许多病毒(包括SARS、MERS 和流感)对人类具有致病性,相关研究具有重要的临床意义。包膜病毒是由外部的包膜包裹遗传物质组成,包膜用于保护病毒,并在病毒感染中发挥重要作用(例如,促进宿主细胞识别和进入)。病毒包膜由脂质和糖蛋白的网状结构组成。包膜的脂质成分不仅对病毒的结构完整性很重要,在促进病毒传播过程的功能方面也起着不可或缺的作用。表征脂质成分是进一步了解病毒包膜在感染过程中的结构和功能作用的关键。所以需要一种高通量表征包膜脂质组成的分析方法。为此,我们使用常压(AP)基质辅助激光解吸电离(MALDI)与高分辨质谱(HRMS)相结合,快速、有效地从包膜病毒中提取检测总脂质。AP-MALDI 减少了使用专用 MALDI 质谱仪的依赖性,并允许将 MALDI 源连接到具有所需特征的质谱仪,其中包括高质量分辨率(>100000)和串联质谱。此外,AP-MALDI 不需要真空源,可在 ESI 和 MALDI 源之间快速转换,由于无需真空设置可加快分析时间。AP-MALDI 结合优化的 MALDI 基质系统,即2',4',6'-三羟基乙酮(THAP)加锂,从而形成了一个强大、高通量的脂质检测平台,特别适合于鞘磷脂检测。我们开发的应用包括甲型流感病毒和 SARS-CoV-2病毒粒子的病毒包膜脂质的结构表征。总的来说,使用 AP-MALDI 与高分辨率质谱结合掺锂基质系统,是一个高通量的分析平台,可用于包膜病毒总脂质提取物的检测和结构表征。
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We have developed a shotgun lipidomics platform, referred to as “multi-dimensional mass spectrometry-based shotgun lipidomics (MDMS-SL)” by exploring a variety of chemical/physical properties of lipids. Recently, this technology has been extended to analyze many classes of low abundance lipids, such as fatty acid esters of hydroxyl-fatty acids (FAHFA) and branched fatty acids. In the current presentation, MDMS-SL will be briefly summarized, the strategies for enhancing lipid analysis used in MDMS-SL will be discussed, the newly extended methods for analysis of lipid classes in low abundance will be presented, and finally, applications of the newly-developed methods for biological/biomedical research will also be mentioned.我们开发了一种被称为"基于多维质谱的鸟枪法脂质组学(MDMS-SL)"平台,以探索脂质的各种化学和物理特性。最近,这项技术被推广到分析多种低丰度脂质,如羟基脂肪酸(FAHFA)和支链脂肪酸生成的酯类。在本文中,将简要总结 MDMS-SL,讨论 MDMS-SL 中用于增强脂质分析的策略,提出新的低丰度脂质分析方法,最后是新方法在生物与生物医学研究上的应用。
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2021沃特世推出多款原位电离质谱产品:RADIAN ASAP,直接分析型四极杆质谱仪,实时检测,结果立等可知,可用于制药及化工行业中间反应监控;食品打假;毒品及非法物快筛等领域。全新加强版DESI XS,可协同新型MALDI源,配备在全新的20万分辨率的SELECT SERIES MRT新型四极杆飞行时间质谱产品上,将飞行时间质谱与成像技术推到新的高度。
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本次讲座主要介绍岛津直接离子化质谱仪(DPiMS)的原理和技术特点,然后重点介绍DPiMS的特色应用,活体分析、疾病模型和构建等经典应用案例。
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Cholesterol is one of the most abundant lipids in the brain. It is heavily enriched in myelin sheaths which wrap around neurons and also found in plasma membranes of all cell types of the brain. Cholesterol is linked to diseases of aging, particularly neurodegenerative diseases, hence there is considerable interest in the use of mass spectrometry imaging of brain to see if cholesterol levels are disturbed in regions of pathology. Being a neutral molecule cholesterol is less amenable to ionisation than other membrane lipids e.g. phospholipids, and is thus discriminated against in mass spectrometry imaging studies.
Here we report the use of two ambient ionisation technologies AP/MALDI (MassTech) and LESA Plus (Advion) combined with Orbitrap (Thermo Scientific) mass spectrometry to image cholesterol and its metabolites in brain tissue sections (10 μm) at high spatial resolution (10 μm pixel) or at high sensitivity (pg/mg). By application of on-tissue derivatisation we have imaged cholesterol at high spatial resolution by AP/MALDI-MS and MS/MS, while for less abundant metabolites, where it is necessary to perform analysis at much lower resolution (800 μm) to achieve sufficient sensitivity, we have utilised the TriVersa NanoMate with LESA Plus. The advantage of the TriVersa NanoMate is that it allows chromatographic separations after extraction and before ionisation. This is important as many cholesterol metabolites exist as isomers. We demonstrate the application of these technologies on mouse and human brain [1, 2].
胆固醇是脑组织中最丰富的脂质。他们富集在包裹着神经元的髓鞘,也存在于脑组织中所有细胞的细胞质膜中。胆固醇与衰老,特别是神经退行性疾病相关,因此在病理学中,运用质谱成像来分析胆固醇水平在脑组织中的分布引起了广泛的兴趣。胆固醇作为一种中性分子,比其他的细胞膜脂质(如磷脂)更难电离,因此质谱成像研究很少涉及这类分子。
在此,我们将报道两种原位电离技术 AP/MALDI (MassTech公司)和 LESA Plus (Advion公司)与Orbitrap 质谱(Thermo公司)来对脑组织切片(10 μm厚)中的胆固醇及其代谢物进行高空间分辨率(10 μm 分辨率)或高灵敏度(pg/mg)成像。我们使用了组织原位衍生化法对胆固醇进行了 AP/MALDI-MS 和 MS/MS 成像,而对于低丰度的代谢物,我们使用了低分辨率(800 μm)的LESA Plus 来获取足够的灵敏度进行分析。许多胆固醇代谢物都有同分异构体,因此运用LESA Plus技术非常重要,它能够实现在原位萃取后的色谱分离,然后再进行离子化。我们将展示这些技术在鼠脑和人脑中的应用成果。[1, 2]
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生物分析是指分析生物基质中的药物、生物标志物或他们的代谢物。准确可靠的生物分析对于药物研发的每一步决定都至关重要。核酸药物作为一类中等大小的多负电荷聚合物,其生物分析有很大的挑战。本报告介绍目前几种常用的核酸药物生物分析方法,并讨论他们在核酸药物不同研发阶段的应用。
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目前全球已有10个寡核苷酸药物上市(FDA),数百个处于临床研究或临床前研究阶段,在中国有1个寡核苷酸药物上市,多个寡核苷酸药物获批进行临床研究。面对如此快速发展的势头,寡核苷酸药物的生产与质量研究至关重要,尤其是建立科学可靠的质量控制和杂质研究方法更为紧迫。
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精准医学;肿瘤于分子;精准分子诊断技术