“State defining” experiment in chemical kinetics—primary characterization of catalyst activity in a TAP experiment
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- 作者：Shekhtman ; Sergiy O. ; Yablonsky ; Gregory S. ; Gleaves ; John T. ; Fushimi ; Rebecca
- 关键词：Kinetics ; Catalyst characterization ; Pulse-response ; TAP-experiment
- 刊名：Chemical Engineering Science
- 出版年：2003
- 出版时间：November, 2003
- 年：2003
- 卷：58
- 期：21
- 页码：4843-4859
- 全文大小：424 K
文摘
This paper presents a new strategy, “state-by-state transient screening”, for kinetic characterization of states of a multicomponent catalyst as applied to TAP pulse-response experiments. The key idea is to perform an insignificant chemical perturbation of the catalytic system so that the known essential characteristics of the catalyst (e.g. oxidation degree) do not change during the experiment. Two types of catalytic substances can be distinguished: catalyst state substances, which determine the catalyst state, and catalyst dynamic substances, which are created by the perturbation. The general methodological and theoretical framework for multi-pulse TAP experiments is developed, and the general model for a one-pulse TAP experiment is solved. The primary kinetic characteristics, basic kinetic coefficients, are extracted from diffusion–reaction data and calculated as functions of experimentally measured exit-flow moments without assumptions regarding the detailed kinetic mechanism. The new strategy presented in this paper provides essential information, which can be a basis for developing a detailed reaction mechanism. The theoretical results are illustrated using furan oxidation over a VPO catalyst.