Acidity and Mechanism in Reactions Catalyzed By Strong Acid Catalyst, Solid and Liquid

本提案的目的是发展一致的方法来确定固体酸性催化剂的酸性功能。本文提出了三个组成部分：通过线性醚络合评价刘易斯酸度，通过吸附吡啶衍生物检查Bronsted位点，以及探索与饱和烃对话相关的反应机制。一个方面将是发展路易斯酸度的定量标度，以醚为碱，核磁共振为探针。酸强度对局部曲率的依赖性已经被观察到，并将被研究。除了在较高温度下通过平衡测量校准酸强度外，还将研究在较低温度下碳氢化合物在沸石上的反应，其中热活化不太重要。所选择的反应物，石蜡和环石蜡，是那些需要最大强度的催化剂进行酸催化反应。这项工作将有助于对一些新一代固体酸，如氧化锆支持的硫酸盐和杂多酸，有更清晰、更基本的了解。

The objective of this proposal is to develop consistent methods for determining the acidity functions of solid acid catalysts. Three components are proposed: evaluation of Lewis acidity by complexation of linear ethers, examination of Bronsted sites by adsorption of pyridine derivatives, and exploration of reaction mechanisms associated with conversation of saturated hydrocarbons. One aspect will be the development of a quantitative scale for Lewis acidity using ethers as bases and nuclear magnetic resonance as the probe. The dependence of acid strength on local curvature has been observed and will be investigated. In addition to a calibration of acid strength from equilibrium measurements as higher temperatures, reactions of hydrocarbons on zeolites at lower temperatures, where thermal activation is less important, will be studied. The reactants chosen, paraffins and cycloparaffins, are those that require the greatest strength of catalyst for an acid-catalyzed reaction. This work will help provide a clearer, fundamental understanding of some newer-generation solid acids such as zirconia-supported sulfates and heteropolyacids.