Analysis of Acid Catalyzed Reaction using Isotopic Transient Kinetics

摘要提案标题：使用同位素瞬态动力学分析酸催化反应提案编号：CTS-9988412首席研究员：James Goodwin机构： 本计画的目的是利用同位素瞬态动力学分析（ITKA）来获得固体酸催化剂动力学参数的原位信息。 这项工作将集中在确定的性质，高活性和选择性的硫酸化氧化锆（SZ）催化剂的丁烷异构化，一个模型反应。 研究的参数将包括平均停留时间和浓度的活性表面中间体，导致异丁烷在正丁烷异构化SZ和过硫酸化氧化锆催化剂。XPS、FTIR、NMR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位点的性质，以便未来催化剂上的位点可以更精确地定制。 在进行更合理的设计之前，需要回答关于SZ催化剂的几个具体问题。 目前还不清楚为什么过硫酸化氧化锆，含有较低浓度的硫酸盐，给出较高的活性正丁烷异构化。 也不清楚为什么氧化铝促进的催化剂促进焦炭形成，但也具有更好的催化剂稳定性。 成功的固体酸催化剂将取代液体酸催化剂，液体酸催化剂会导致腐蚀、催化剂分离以及来自酸循环和处置的环境问题。

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.