High-Resolution Ion Mobility Mass Spectrometer for Complex Mixture Analysis

质谱仪(MS)是最强大的分析技术之一。特别是，高分辨MS(HRMS)已经成为提供环境科学、代谢组学、蛋白质组学、石油组学和法医学等不同学科中复杂分子体系的深入化学组成知识的不可或缺的技术。从21世纪初开始，主要使用傅里叶变换质量分析仪(Orbitrap和傅里叶变换离子回旋加速器)。然而，尽管分辨率在1e5以上、质量精度低于ppm的超高分辨率MS提供了准确的元素组成数据，但它在揭示结构信息方面存在局限性。因此，经常使用连接的溶液，例如层析耦合或碎裂和解离方法。在过去的十年中，几种离子迁移率质谱仪(IMS-MS)相继问世。简而言之，离子迁移率光谱沿着电场和气流梯度按大小和形状分离离子。因此，作为分离和分辨的附加维度，增加了碰撞横截面这一固有的结构属性。这项建议旨在通过将高分辨率离子迁移率光谱与高分辨率MS相结合，使最先进的IMS-MS平台达到超高峰容量。飞行时间质量分析仪固有的有限分辨率将通过以下方式克服：A)利用现有的选择性电离概念，如电喷雾和大气压化学电离，B)开发新的选择性和灵敏的光电离化方案，以及C)通过热分析、气相色谱和高效液相色谱连接第四维分离。该平台将解决以下领域的研究问题和现代分析发展需求：1)环境科学--来自各种健康和环境相关排放源的初级和次级有机气溶胶；2)气溶胶毒理学和诱变--化学成分和代谢组学生物标记物的联系；3)材料科学--循环经济背景下的生物油和回收利用。4)海洋科学--水溶和天然有机物，5)医学研究--人体肠道和胃肠病学，6)仪器开发--使用所建议仪器的MALDI能力的新型联用和光电离化方案。拟议的基础设施旨在为复杂混合物的直接分析提供现代质谱学能力，不仅在元素组成水平上提供有价值的见解，而且在环境、医学、生物和能源转换研究中提供结构信息。通过弥合化学成分和结构洞察之间的差距，这个平台将促进对复杂混合物中化合物的环境命运、化学反应以及毒理学和代谢组学潜力的研究。

Mass spectrometry (MS) is one of the most powerful analytical techniques. In particular, high-resolution MS (HRMS) has become an indispensable technique providing in-depth chemical composition knowledge on complex molecular systems in diverse disciplines, such as environmental sciences, metabolomics, proteomics, petroleomics, and forensic sciences. From the early 2000s, primarily Fourier-transform mass analyzer (Orbitrap and Fourier-transform ion cyclotron) have been used. However, while ultra-high-resolution MS with resolving power above 1e5 and sub-ppm mass accuracy provides accurate elemental composition data, it has limitations in revealing structural information. Consequently, hyphenated solutions, such as chromatography coupling, or fragmentation and dissociation approaches, are frequently deployed. In the last decade, several ion mobility mass spectrometers (IMS-MS) were commercially introduced. Briefly, ion mobility spectrometry separates ions by size and shape along an electrical field and gas flow gradient. Hereby, the collision-cross section, an intrinsic structural property, is added as additional dimension of separation and resolution. This proposal aims for a state-of-the-art IMS-MS platform reaching ultra-high peak capacities by combining high-resolution ion mobility spectrometry with high-resolution MS. The inherent limited resolving power of the time-of-flight mass analyzer will be overcome by A) utilizing existing selective ionization concepts, such as electrospray and atmospheric pressure chemical ionization, B) development of novel selective and sensitive photoionization schemes, and C) by hyphenation of a 4th dimension separation via thermal analysis, gas chromatography and high-performance liquid chromatography. The platform will allow addressing research questions and modern analytical development needs from the following fields: 1) Environmental Sciences - Primary and Secondary Organic Aerosols from various Health and Environmental Relevant Emission Sources, 2) Aerosol Toxicology and Mutagenesis - Linkage of Chemical Composition and Metabolomics Biomarkers, 3) Material Sciences - Bio-oils and Recycling within the Circular Economy Context. 4) Marine Sciences - Aquatic Dissolved and Natural Organic Matter, 5) Medical Research - Human Intestine and Gastroenterology, 6) Instrumental Development - Novel Hyphenation and Photoionization Schemes using the MALDI capability of the proposed instrument. The proposed infrastructure aims to provide modern mass spectrometric capabilities for direct analysis of complex mixtures, offering valuable insights not only at the elemental composition level but also structural information in environmental, medical, biological, and energy transition research. By bridging the gap between chemical composition and structural insights, this platform will facilitate investigations into the environmental fate, chemical reactivity, and toxicological and metabolomics potential of compounds in complex mixtures.