Kinetics and Mechanism of the Hydrolysis and Rearrangement Processes within the Assembly-Disassembly-Organization-Reassembly Synthesis of Zeolites

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作者
Henkelis, Susan E. [1 ]
Mazur, Michal [2 ]
Rice, Cameron M. [1 ]
Wheatley, Paul S. [1 ]
Ashbrook, Sharon E. [1 ]
Morris, Russell E. [1 ,2 ]
机构
[1] School of Chemistry and EaStCHEM, University of St. Andrews, North Haugh, St.Andrews-Fife,KY16 9ST, United Kingdom
[2] Department of Physical and Macromolecular Chemistry, Faculty of Sciences, Charles University, Hlavova 8, 2, Prague,128 43, Czech Republic
来源
Journal of the American Chemical Society | 2019年
基金
欧盟地平线“2020”;
关键词
Activation energy - Hydrolysis - Temperature - Kinetics;
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学科分类号
摘要
The hydrolysis (disassembly, D) and rearrangement (organization, O) steps of the assembly-disassembly-organization-reassembly (ADOR) process for the synthesis of zeolites have been studied. Germanium-rich UTL was subjected to hydrolysis conditions in water to understand the effects of temperature (100, 92, 85, 81, 77, and 70 °C). Samples were taken periodically over an 8-37 h period, and each sample was analyzed by powder X-ray diffraction. The results show that the hydrolysis step is solely dependent on the presence of liquid water, whereas the rearrangement is dependent on the temperature of the system. The kinetics have been investigated using the Avrami-Erofeev model. With increasing temperature, an increase in the rate of reaction for the rearrangement step was observed, and the Arrhenius equation was used to ascertain an apparent activation energy for the rearrangement from the kinetic product of the disassembly (IPC-1P) to the thermodynamic product of the rearrangement (IPC-2P). From this information, a mechanism for this transformation can be postulated. © Copyright 2019 American Chemical Society.
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