线性升高的环境温度对封闭系统中放热反应的影响

T. Boddington, P. Gray, S. R. Kay
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引用次数: 4

摘要

一般来说,热分析,特别是差示扫描量热法,为研究放热分解提供了快速和自动化的技术。当反应不太复杂时,可以提取放热量和阿伦尼乌斯参数的值。大多数数学处理的基础并不深入,而且通常依赖于对“静态”情况的分析,其中对恒定环境温度的响应是起点。本文对反应样品连续加热的动态过程进行了经济分析。热爆炸理论的约化变量提供了一个符合一阶速率定律的单一反应的标准情况的紧凑表示,它与阿累尼乌斯温度有关。采用渐近处理方法将质量守恒方程和能量守恒方程细化为具有实际意义的形式。以这种方式产生的自然变量导致了以化学反应速率而不是更常见的样品温度为依据的系统模型。这种新的处理方法对所有有用的操作条件下的反应行为进行了清晰而紧凑的描述。通常由静态处理得出的著名的基辛格关系被认为与这个模型有关,但必须小心选择与之相关的精确物理量。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
The effects of a linearly increasing ambient temperature on an exothermic reaction in a closed system
Thermal analysis in general, and differential scanning calorimetry in particular, offer rapid and automated techniques for studying exothermic decompositions. When reaction is not too complex, values for the exothermicities and Arrhenius parameters may be extracted. The basis of most mathematical treatments is not deep and quite commonly rests on analyses of ‘static’ situations, in which the responses to constant ambient temperatures are the starting point. In this paper we give an economical analysis of the dynamic process of heating a reactive sample continuously. The reduced variables of thermal explosion theory provide a compact representation of the standard case of a single reaction obeying a first-order rate law with an Arrhenius temperature dependence. An asymptotic treatment is used to refine the equations of mass and energy conservation to a practically important form. The natural variables that arise in this way lead to a model of the system in terms of the rate of the chemical reaction, rather than the more usual temperature of the sample. This new treatment leads to a clear and compact description of the behaviour of the reaction for all useful operating conditions. The well-known Kissinger relation normally derived from static treatments is seen to be relevant in this model, but care must be taken in choosing the precise physical quantities to which it relates.
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