High-Resolution Ion Mobility Mass Spectrometer for Complex Mixture Analysis

质谱（MS）是最强大的分析技术之一。特别是，高分辨率质谱（HRMS）已成为一种不可或缺的技术，提供深入的化学组成知识的复杂分子系统在不同的学科，如环境科学，代谢组学，蛋白质组学，石油组学和法医科学。从21世纪初开始，主要使用傅里叶变换质量分析仪（轨道阱和傅里叶变换离子回旋加速器）。然而，虽然分辨率高于1 e5和亚ppm质量精度的超高分辨率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，联用的解决方案，如色谱耦合，或碎片和解离的方法，经常部署。在过去的十年中，商业上引入了几种离子迁移率质谱仪（IMS-MS）。简而言之，离子迁移谱法通过尺寸和形状沿着电场和气流梯度分离离子。因此，碰撞截面，一个内在的结构特性，被添加作为额外的维度的分离和分辨率。该提议旨在通过将高分辨率离子迁移谱与高分辨率MS相结合来实现达到超高峰容量的最先进的IMS-MS平台。飞行时间质量分析器的固有有限分辨能力将通过以下方式来克服：A）利用现有的选择性电离概念，例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方案，和C）通过热分析、气相色谱和高效液相色谱的第四维分离的联用。该平台将允许解决以下领域的研究问题和现代分析开发需求：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志物的联系，3）材料科学-循环经济背景下的生物油和回收。4)海洋科学-水生溶解和天然有机物，5）医学研究-人类肠道和胃肠病学，6）仪器开发-使用拟议仪器的MALDI能力的新连字符和光电离方案。拟议的基础设施旨在提供现代质谱能力，用于直接分析复杂混合物，不仅在元素组成水平上提供有价值的见解，而且还在环境，医学，生物和能源转型研究中提供结构信息。通过弥合化学组成和结构洞察之间的差距，该平台将促进对复杂混合物中化合物的环境归宿、化学反应性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.