Development and application of novel ionisation sources for mass spectrometry/ biological chemistry

生物分子如碳水化合物、脂质、由于植物和动物来源的蛋白质和核酸存在于复杂的基质中，因此通过质谱分析它们可能具有挑战性。环境解吸/电离（ADI）质谱领域提供了分析其中一些化合物的可能性，这些化合物需要有限的样品制备或不需要样品制备。为了解决这些挑战，下一代紧凑型等离子体ADI源基于流动余辉模式设计中的大气压辉光放电，将开发用于质谱分析的辉光流（GlowFlow）。该源将是工程师，使其具有良好的灵敏度作为一种定性分析方法，保留了一个大得多，但笨重的原型的特点。它将被设计为一个通用接口，用于一系列质谱仪和样品入口，解决现有设计中缺乏可识别接口和可重复性的问题。该源将用于研究气相离子分子反应，这些反应的特征机制将用于研究合适的掺杂剂，以进一步提高源的电离效率。由于等离子体放电中发生的电离过程的范围，与更传统的源相比，该源将适合于分析从极性到非极性的各种样品化学物质。该源电离各种样品化学物质的能力及其高灵敏度意味着它将在生物化学以及小分子药物，农药，爆炸物和滥用药物。质谱市场预计到2022年将增长到超过50亿美元，由于其紧凑的设计和与一系列入口的集成，这种新的基于等离子体的源具有在下一代仪器中商业化的潜力。研究方向：分析科学化学生物学与生物化学化学反应动力学与机理化学结构

The analysis of biomolecules such as carbohydrates, lipids, proteins and nucleic acid form plant and animal sources by mass spectrometry can be challenging due to the complex matrices in which they are found. The field of ambient desorption/ionisation (ADI) mass spectrometry offers the possibility to analyse some of these compounds requiring limited or no sample preparation.To address these challenges a next generation compact plasma ADI source (termed GlowFlow) for mass spectrometry will be developed based on the atmospheric pressure glow discharge in the flowing afterglow mode design. The source will be to engineer so that it has good sensitivity as a qualitative analysis method, retaining the characteristics of a much larger but cumbersome prototype. It will be designed with a universal interface for a range of mass spectrometers and sample inlets addressing the lack of recognisable interfaces and reproducibility of existing designs.The source will be used to study gas phase ion-molecule reactions and the characterised mechanisms of these reactions will be used to investigate suitable dopants to further enhance the source's ionisation efficiency. Due to the range of ionisation processes occurring in the plasma discharge the source will be suitable for the analysis of a wide range of sample chemistries' from polar to non-polar when compared to more conventional sources.The source's ability to ionise a wide range of sample chemistries and its high sensitivity means it will find particular application in biological chemistry, as well as for small molecule pharmaceuticals, pesticides, explosives, and drugs of abuse. The mass spectrometry market is estimated to grow to over US$5 billion by 2022 and due to its compact design and integration with a range of inlets this new plasma-based source has the potential for commercialisation in the next generation of instruments. EPSRC Research Areas:Analytical scienceChemical biology and biological chemistryChemical reaction dynamics and mechanismsChemical structure