GOALI: Gas-Phase Reactions of Neutral Organic Molecules Desorbed by Laser-Induced Acoustic Waves

目标：激光诱导声波解吸中性有机分子的气相反应

• 批准号: 0092119
• 负责人: Hilkka Kenttamaa
• 金额: $ 31.05万
• 依托单位: Purdue University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2001
• 资助国家: 美国
• 起止时间: 2001-06-15 至 2004-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0092119&HistoricalAwards=false
• 关键词: GOALI; Gas; Phase; Reactions; Neutral

With this GOALI award, the Organic and Macromolecular Chemistry Program in the Chemistry Division and the MPS Office of Multidisciplinary Activities supports the work of Dr. Hilkka I. Kenttamaa of the Department of Chemistry at Purdue University in West Lafayette, Indiana and Dr. David Aaserud of the Lubrizol Corporation. A high-risk/high-gain research project involving Purdue University and Lubrizol Corporation is proposed for the study of optoacoustic desorption as a means to evaporate neutral molecules into mass spectrometers. The goal is to determine whether the combination of laser-induced acoustic desorption (LIAD) with gas-phase ion-molecule reactions involving mass-selected reagent ions provides benefits in mass spectrometric characterization of thermally labile and/or nonvolatile molecules. Preliminary experiments confirm the feasibility of the concept, demonstrate high predictability and reproducibility, and suggest some intriguing possibilities. For example, the ability to bring neutral (not ionic) nonvolatile and/or thermally labile molecules into the gas phase would allow a variety of fundamental thermochemical, structural and reactivity studies that currently cannot be carried out. Further, this simple approach may provide an attractive complement to MALDI in qualitative analysis. A matrix should not be necessary, which may lead to better predictability. The physical separation of the evaporation and ionization events should permit the use of many different types of ionization reactions, thus providing control over reaction products and thermochemistry, and access to a variety of information for a given analyte. Finally, this approach should allow mass spectrometric characterization of some compounds that are currently not amenable to such analysis.Dr. David Aaserud, the Co-PI on the award, will commit 5-10% of his time and resources to the proposed work where he will jointly advise participating graduate students and provide polymer characterization expertise to the project. Interaction will include monthly progress reviews and the supervision of one or two doctoral students during work at Lubrizol. The students will be exposed to Lubrizol's analytical capabilities and to an industrial environment. Lubrizol will provide relevant samples and access to any appropriate additional analytical information, including GPC, LC, and NMR data. In the technology transfer stage, the laboratories at Lubrizol will be accessible for applications of the new technologies to industrial samples. The Lubrizol Corporation has provided financial support to graduate students and research projects in Professor Kenttamaa's laboratory over several years. Lubrizol is committed to continue this funding as part or their cost sharing. Lubrizol views the collaborative effort as a continuation of its interaction with Professor Kenttamaa's group with a significant increase in the commitment of resources.The proposed research is at the frontiers of mass spectrometry in studies of the selective transfer of molecules from the solid phase to the gas phase. Lubrizol's interest in derivatized polyalphaolefins arises from the fact that these substances are important components of many lubricant additives. The development of new and better methods to characterize hydrocarbon polymers and their functionalized derivatives will allow a better understanding of these materials and help Lubrizol to better predict product performance. With the support of the Organic and Macromolecular Chemistry Program and the MPS Office of Multidisciplinary Activities, the PI is able to perform potentially ground-breaking research as well as work with an industrial partner to explore real-world applications of the research. Professor Kenttamaa has a large group of undergraduate and graduate students who are female or from underrepresented groups. For them the research is expected to provide a valuable educational experience.

有了这个GOALI奖，化学部的有机和高分子化学计划和多学科活动的MPS办公室支持博士的工作。位于印第安纳州西拉斐特的普渡大学化学系的Albertamaa博士和路博润公司的大卫Aaserud博士。普渡大学和路博润公司提出了一个高风险/高收益的研究项目，用于研究光声解吸作为一种手段，蒸发中性分子进入质谱仪。我们的目标是确定激光诱导声解吸（LIAD）与气相离子分子反应，涉及质量选择的试剂离子的组合是否提供的好处，热不稳定和/或非挥发性分子的质谱表征。初步实验证实了这一概念的可行性，表现出高度的可预测性和可重复性，并提出了一些有趣的可能性。例如，将中性（非离子）非挥发性和/或热不稳定分子带入气相的能力将允许目前无法进行的各种基本热化学，结构和反应性研究。此外，这种简单的方法可以提供一个有吸引力的补充MALDI在定性分析。不应该需要矩阵，这可能会带来更好的可预测性。蒸发和电离事件的物理分离应允许使用许多不同类型的电离反应，从而提供对反应产物和热化学的控制，并获得给定分析物的各种信息。最后，这种方法应该允许质谱表征的一些化合物，目前还不适合这样的分析。博士大卫Aaserud，对该奖项的合作PI，将承诺他的时间和资源的5-10%的拟议工作，他将共同建议参与研究生和提供聚合物表征的专业知识，该项目。互动将包括每月进度回顾以及在路博润工作期间对一至两名博士生的监督。学生将接触到路博润的分析能力和工业环境。路博润将提供相关样品并提供任何适当的附加分析信息，包括GPC、LC和NMR数据。在技术转让阶段，路博润的实验室可将新技术应用于工业样品。多年来，路博润公司一直在为研究生和Albertamaa教授实验室的研究项目提供资金支持。路博润承诺将继续提供这笔资金，作为其成本分摊的一部分。路博润将此次合作视为其与Littamaa教授团队互动的延续，并将大幅增加资源投入。拟议的研究处于质谱法研究分子从固相到气相的选择性转移的前沿。路博润之所以对衍生聚α烯烃感兴趣，是因为这些物质是许多润滑油添加剂的重要成分。开发新的、更好的方法来表征烃类聚合物及其官能化衍生物，将有助于更好地了解这些材料，并帮助路博润更好地预测产品性能。在有机和高分子化学计划和多学科活动的MPS办公室的支持下，PI能够进行潜在的突破性研究，并与工业合作伙伴合作，探索研究的实际应用。Albertamaa教授有一大批本科生和研究生，她们都是女性或来自代表性不足的群体。对他们来说，这项研究有望提供宝贵的教育经验。