Kinetic effects of pressure on decomposition of solids

IF 2.5 2区 化学 Q3 CHEMISTRY, PHYSICAL International Reviews in Physical Chemistry Pub Date : 2020-01-02 DOI:10.1080/0144235X.2019.1691319
S. Vyazovkin
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引用次数: 36

Abstract

The kinetics of thermal decomposition of solids is discussed in connection with three major approaches to inducing pressure: by manipulating pressure of the product gas, by changing pressure of an inert gas, and by applying a mechanical force. The first two approaches are implemented in differential scanning calorimetry (DSC) and thermogravimetry (TGA), whose upper pressure limit is in the MPa range. The third approach is implemented in diamond anvil cells that extend measurements to the GPa range. In the GPa range a response of the rate to pressure is determined by the sign of the activation volume change. In the MPa range this response is determined by pressure of the gaseous product in the reaction zone. Manipulating the product gas pressure affects directly the kinetics of reversible decompositions as described by a number of models. Changing pressure of an inert gas results in indirect manipulation of pressure of the gaseous products that can engage in reaction with the reactant or another product and thus affect the kinetics of autocatalytic and reversible decompositions. These and other effects are discussed with the emphasis on changes in the activation energy and preexponential factor as a function of pressure, temperature, and conversion.
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压力对固体分解的动力学影响
讨论了固体热分解动力学与诱导压力的三种主要方法:通过操纵产物气体的压力,通过改变惰性气体的压力,以及通过施加机械力。前两种方法在差示扫描量热法(DSC)和热重法(TGA)中实现,其压力上限在MPa范围内。第三种方法是在金刚石砧单元中实现,将测量范围扩展到GPa范围。在GPa范围内,速率对压力的响应由活化体积变化的符号决定。在MPa范围内,这种反应是由反应区内气体产物的压力决定的。正如许多模型所描述的那样,操纵产物气体压力直接影响可逆分解的动力学。改变惰性气体的压力导致间接操纵气体产物的压力,这些气体产物可以与反应物或其他产物发生反应,从而影响自催化和可逆分解的动力学。讨论了这些和其他影响,重点讨论了活化能和指前因子作为压力、温度和转化率的函数的变化。
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来源期刊
CiteScore
14.20
自引率
1.60%
发文量
5
审稿时长
1 months
期刊介绍: International Reviews in Physical Chemistry publishes review articles describing frontier research areas in physical chemistry. Internationally renowned scientists describe their own research in the wider context of the field. The articles are of interest not only to specialists but also to those wishing to read general and authoritative accounts of recent developments in physical chemistry, chemical physics and theoretical chemistry. The journal appeals to research workers, lecturers and research students alike.
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