第 IX 章.非等温链式过程的动力学规律

IF 16.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
V. V. Azatyan
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引用次数: 0

摘要

摘要 强调了反应速率和速率常数的温度依赖性之间很少被考虑到的根本区别。与现有观点相反,高活化能反应的速率变化很小。研究表明,计算速率与实验速率之间出现偏差的主要原因是忽略了反应过程中试剂浓度的温度依赖性。结果表明,计算速率值和实验速率值之间出现偏差的主要原因是忽略了反应过程中反应物浓度的温度依赖性。引入了温度速率常数的概念:单位温度变化时的速率变化,即速率常数的温度导数。研究表明,这一特性决定了非等温条件下复杂过程各阶段之间的竞争。发现了链式过程的温度依赖定律,并验证了其与实验的一致性。解释了温度升高和活性粒子增殖引起的反应自加速之间的区别。并提供了实验说明。解释了点火前后从外部加热的气体中反应速率随温度变化的差异。根据实验数据,定量证明了氢原子浓度在百分之一大气压和大气压下对燃烧速率的决定作用。这证明了初始试剂焓的很大一部分转化为自由价能对燃烧的决定作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Chapter IX. Laws of Kinetics of Nonisothermal Chain Processes

Chapter IX. Laws of Kinetics of Nonisothermal Chain Processes

Chapter IX. Laws of Kinetics of Nonisothermal Chain Processes

The rarely considered fundamental difference between the temperature dependences of the reaction rate and the rate constant is emphasized. The small change in the rate of reactions with high activation energies, contrary to existing ideas, is illustrated. It was shown that the main reason for the deviation between the calculated and experimental rates is the neglect of the temperature dependence of the reagent concentrations during the reaction. It has been shown that the main reason for the deviation between the calculated and experimental rate values is the neglect of the temperature dependence of the reactant concentrations in the course the reaction. The concept of the temperature rate constant is introduced: the change in the rate with a unit change in temperature, i.e., the temperature derivative of the rate constant. It is shown that this characteristic determines the competition between the stages of a complex process under nonisothermal conditions. The law of temperature dependence of the chain process was discovered, and its agreement with experiment was verified. The difference between the self-acceleration of a reaction from an increase in temperature and from the multiplication of active particles is explained. An experimental illustration is provided. The difference between the temperature dependences of the reaction rates in a gas heated from outside before and after the onset of ignition is explained. Based on experimental data, the determining role of the hydrogen atom concentrations in the combustion rate at hundredths of atmospheric pressure and at atmospheric pressure is quantitatively demonstrated. This demonstrates the determining role in combustion of the conversion of a significant part of the enthalpy of the initial reagents into the free-valence energy.

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来源期刊
Accounts of Chemical Research
Accounts of Chemical Research 化学-化学综合
CiteScore
31.40
自引率
1.10%
发文量
312
审稿时长
2 months
期刊介绍: Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.
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