Theory of Chemical Reactions in Solution, in Clusters, and at Surfaces

溶液、团簇和表面的化学反应理论

• 批准号: 9700419
• 负责人: James Hynes
• 金额: $ 32.91万
• 依托单位: University of Colorado at Boulder
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1997
• 资助国家: 美国
• 起止时间: 1997-06-01 至 2001-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9700419&HistoricalAwards=false
• 关键词: Theory; Chemical; Reactions; Solution; Clusters

James Hynes of the Chemistry Department of the University of Colorado is funded by the Physical Chemistry Program of the Chemistry Division to study the kinetic theory of prototype reactions in solutions, small clusters and at surfaces. Quantitative predictions and qualitative interpretations will be provided for experiments. The calculations will be carried out using quantum electronic structure methods, molecular dynamics, analytic theories and models. The solution phase research will focus in two areas: (1) Excited photon transfer reactions (ESPT) in which acidity is dramatically increased by photoexcitation. (2) Reaction dynamics in electrolytes. The dynamics of prototype unimolecular SN1 ionization reaction of tertiary butyl chloride in salt solutions will be studied. Furthermore, heterogeneous surface chemical reactions responsible for the depletion of the ozone in the upper atmosphere will be investigated. By far the majority of reactions which are of interest to chemists take place in the solution phase, and the most important solvent is water. The effect which the presence of aqueous solvent has on a chemical reaction is still not fully understood. Hynes is applying a combination of theory and computer simulations to determine the molecular nature of solvent-solute interactions and their effect on the rates of chemical reactions in solution. He is also applying these theoretical methods to studies of important environmental problems such as acid rain and ozone depletion.

科罗拉多大学化学系的詹姆斯·海恩斯（James Hynes）由化学部的物理化学计划资助，用于研究解决方案，小簇和表面中原型反应的动力学理论。 实验将提供定量预测和定性解释。计算将使用量子电子结构方法，分子动力学，分析理论和模型进行。溶液相研究将集中在两个领域：（1）激发光子转移反应（ESPT），其中酸度通过光激发大大增加。 （2）电解质中的反应动力学。将研究盐溶液中第三级丁基氯化物的原型非分子SN1离子化反应的动力学。此外，将研究负责上层大气中臭氧耗竭的异质表面化学反应。 到目前为止，化学家感兴趣的大多数反应都是在溶液阶段发生的，最重要的溶剂是水。 水溶液的存在对化学反应的影响仍未完全了解。 Hynes正在应用理论和计算机模拟的组合来确定溶剂 - 溶液相互作用的分子性质及其对溶液中化学反应速率的影响。 他还将这些理论方法应用于重要的环境问题，例如酸雨和臭氧消耗。