Desorption/Ionization in Nanofiber SALDI Mass Spectrometry

在化学系化学测量和成像计划的支持下，俄亥俄州立大学的Susan Olesik博士和Zachary Schultz博士及其团队正在努力改进表面辅助激光解吸电离(SALDI)质谱仪，这是一种同时检测小化学物种和大分子(如聚合物和蛋白质)的强大分析方法。从这项工作中获得的见解应该能够加强环境分析，例如监测自然水域中微量污染物的数量，并通过跟踪越来越低水平的生物流体中与疾病有关的物种来检测人类疾病。为了增加历史上代表性不足的学生在科学领域的机会，如第一代大学生和少数族裔，两个研究小组的招聘努力将允许这些本科生与各自实验室的研究生一起工作，获得最先进的实验室科学技能。Olesik和Schultz团队正在致力于通过对激发激光和Saldi衬底之间、衬底内部以及从衬底到分析物分子之间的能量转移的基础研究，来改进基于纳米纤维的表面辅助激光解吸/电离SALDI的性能。这项工作的首要目标是显著提高基于纳米纤维的SALDI的性能。与基质辅助激光解吸电离相比，SALDI通常为小分子的分析提供了显著的优势，因为MALDI的检测下限较低，提高了质谱图中信号/噪声的重现性，并且在由于基质电离而产生的低质量范围内不存在“化学”背景。基于纳米纤维的SALDI具有其他实现的所有优点；然而，它也经常可以对特定的高分子量化合物实现强信号/噪声。基于纳米纤维的SALDI的性能将通过对激发激光和SALDI衬底之间、衬底内以及从衬底到分析物分子的能量转移的基础研究来改进。这项关于能量转移如何影响基于纳米纤维的SALDI的解吸/电离的机械研究预计将定义适用于低分子分析和高分子分析的痕量检测的高性能结构。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Drs. Susan Olesik and Zachary Schultz and their groups at Ohio State University are working to improve on Surface-Assisted Laser Desorption Ionization (SALDI) mass spectrometry, a powerful analytical method for the detection of both small chemical species and large macromolecules (e.g.- polymers and proteins). Insights gained in this work should enable enhanced environmental analyses, such as monitoring trace-level amounts of pollutants in natural waters and human disease detection through tracking disease-related species in biological fluids at increasingly low levels. To enhance the opportunities for historically underrepresented students in science, such as first generation college students and racial minorities, recruitment efforts by both research groups will allow these undergraduates to work alongside graduate students in the respective laboratories to acquire skills in state-of-the art laboratory science. The Olesik and Schultz group are working to improve the performance of nanofiber-based surface assisted laser desorption/ ionization, SALDI, through fundamental studies of energy transfer between the excitation laser and the SALDI substrate, within the substrate, and from the substrate to the analyte molecules. The overarching goal of this work is to markedly enhance the performance of nanofiber-based , SALDI. Often SALDI provides significant advantages for analysis of small molecules compared to matrix-assisted laser desorption ionization, MALDI, due to the low detection limits, improved reproducibility of signal/noise in the mass spectrum, and the absence of a “chemical” background in the low mass range arising from ionization of the matrix. Nanofiber-based SALDI has all the advantages of other implementations; however, it can also often achieve strong signal/noise for specific high molecular weight compounds. The performance of nanofiber based SALDI will be improved through fundamental studies of energy transfer between the excitation laser and SALDI substrate, within the substrate, and from the substrate to the analyte molecules. This mechanistic study of how energy transfer impacts desorption/ionization for nanofiber-based SALDI is expected to define high performing constructs appropriate for trace detection of both low and high molecular weight analytes.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.