Analysis of Acid Catalyzed Reaction using Isotopic Transient Kinetics

摘要题目：用同位素瞬时动力学分析酸催化的反应提议编号：CTS-9988412主要研究人员：詹姆斯·古德温研究所：匹兹堡大学这个项目的目标是使用同位素瞬时动力学分析(ITKA)来获得固体酸催化剂动力学参数的现场信息。这项工作将集中在确定硫化氧化锆(SZ)催化剂对丁烷异构化的高活性和选择性的性质，这是一个模型反应。所研究的参数包括正丁烷异构化过程中活性表面中间体在SZ和过硫化氧化锆催化剂上的平均停留时间和浓度。XPS、FTIR、核磁共振和微量热法等分析技术将补充ITKA研究。这项工作的总体目标是了解活性中心的性质，以便未来催化剂上的中心可能更精确地定制。在进行更合理的设计之前，需要回答几个关于SZ催化剂的具体问题。目前尚不清楚为什么含有较低浓度硫酸盐的过硫化氧化锆对正丁烷异构化具有较高的活性。目前也不清楚为什么氧化铝促进的催化剂可以促进焦炭的形成，但也具有更好的催化剂稳定性。一种成功的固体酸催化剂将取代液态酸催化剂，这将导致酸回收和处置带来的腐蚀、催化剂分离和环境问题。

AbstractProposal Title: Analysis of Acid Catalyzed Reactions Using Isotopic Transient KineticsProposal Number: CTS-9988412Principal Investigator: James GoodwinInstitution: University of PittsburghThe objective of this project is to use isotopic transient kinetic analysis (ITKA) to obtain in situ information on kinetic parameters for solid acid catalysts. The work will focus on determining the nature of the high activity and selectivity of sulfated zirconia (SZ) catalysts for butane isomerization, a model reaction. Parameters studied will include average residence time and concentration of active surface intermediates leading to iso-butane during n-butane isomerization on SZ and persulfated zirconia catalysts. Analytical techniques such as XPS, FTIR, NMR, and microcalorimetry will complement ITKA studies. An overall goal of this work is to understand the nature of active sites such that the sites on future catalysts might be more precisely tailored. Several specific questions need to be answered about SZ catalysts before more rational design can proceed. It is unclear why persulfated zirconia, containing a lower concentration of sulfate, gives higher activity for n-butane isomerization. It is also unclear why alumina-promoted catalysts promote coke formation but also have better catalyst stability. A successful solid-acid catalyst would replace liquid-acid catalysts, which lead to corrosion, catalyst separation, and environmental problems from acid recycle and disposal.