Spectroscopic Detection and Characterization of Chemical Intermediates

化学中间体的光谱检测和表征

• 批准号: 9320909
• 负责人: Terry Miller
• 金额: --
• 依托单位: Ohio State University Research Foundation -DO NOT USE
• 依托单位国家: 美国
• 项目类别: Continuing grant
• 财政年份: 1994
• 资助国家: 美国
• 起止时间: 1994-03-01 至 1999-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9320909&HistoricalAwards=false
• 关键词: Spectroscopic; Detection; Characterization; Chemical; Intermediates

In this project in the Physical Chemistry Program of the Chemistry Division, Prof. Terry A. Miller of the Ohio State University will conduct fundamental investigations of chemical reaction intermediates and clusters involving them. The primary method for detection and characterization of the species is high resolution spectroscopy. The species are produced in the cold, unreactive environment of a supersonic jet expansion where they can be interrogated by bot moderate and very high resolution laser induced fluorescence (LIF) spectroscopy. Using the same jet techniques, the zero kinetic energy (ZEKE) spectroscopy of the chemically very important ions of a number of reactive, neutral free radicals will be characterized. Specific chemical intermediates to be studied as neutrals and/or cations include alkoxy radicals and their fluoro- and thio-derivatives, carbenes, amiodogen and related radicals, and substituted methyl radicals (carbonium ions). Concurrent theoretical developments in fundamental spectroscopic theory, applied spectroscopic analysis, and ab initio calculations on the chemical intermediates will be undertaken. Complex chemical reactions that occur in atmospheric, combustion, and organic synthesis processes typically involve transient chemical intermediates, such as free radicals and molecular ions, that determine the overall result of the process. Spectroscopic identification of the intermediates is critical for the practical investigation and monitoring of such reactions. Spectroscopic characterization of the intermediates provides a foundation for the basic understanding of the nature of chemical reactivity. This research involves a multifaceted approach to the spectroscopic detection and characterization of these intermediates and species involving them.

在化学系物理化学项目的这个项目中，俄亥俄州立大学的Terry A. Miller教授将对化学反应中间体及其涉及的团簇进行基础研究。 检测和表征物种的主要方法是高分辨率光谱法。 这些物种是在超音速射流膨胀的寒冷、无反应的环境中产生的，在那里它们可以通过机器人中等和超高分辨率激光诱导荧光（LIF）光谱进行询问。 使用相同的喷射技术，将表征许多反应性中性自由基的化学上非常重要的离子的零动能（ZEKE）光谱。 作为中性物和/或阳离子进行研究的具体化学中间体包括烷氧基及其氟代和硫代衍生物、卡宾、胺基和相关基团以及取代的甲基基团（碳正离子）。 将同时进行基础光谱理论、应用光谱分析和化学中间体从头计算的理论发展。 大气、燃烧和有机合成过程中发生的复杂化学反应通常涉及瞬态化学中间体，例如自由基和分子离子，它们决定了该过程的总体结果。 中间体的光谱鉴定对于此类反应的实际研究和监测至关重要。 中间体的光谱表征为基本了解化学反应性的本质提供了基础。 这项研究涉及对这些中间体和涉及它们的物种进行光谱检测和表征的多方面方法。