Chapter III. Specificities of the Mechanism and Energy of Branching Chain Processes

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL
V. V. Azatyan
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Abstract

It is shown that the features of chain processes are determined mainly by the fact that most of the internal energy of the initial reagents is converted into the energy of free valences of atoms and radicals. This results in high concentrations of active particles, which react with the initial reagents at higher rates, providing intensive self-heating, which additionally accelerates the process. It is noted that, without considering the chain nature of reactions, it is impossible to explain ignition upon heating, since the high activation energies of reactions of only molecular reagents exclude an increase in the rate during heating. Taking into account the chain nature of combustion reactions made it possible to explain ignition upon heating and develop a theory of the phenomenon. An explanation is given to the most important characteristic of gas combustion: the length of reaction chains, which determines the role of the chain mechanism in combustion, and the dependence of kinetics on temperature. A solution to the problems of the third flammability limit, confirmed by kinetic and spectroscopic experiments, was obtained, as well as the evidence of the presence of HO2 radicals in the flame, their active role in the heterogeneous development of reaction chains and in combustion in general. The possibility of replacing the solution of diffusion differential equations by effective kinetic parameters when describing combustion has been experimentally proven.

Abstract Image

Abstract Image

第 III 章.支链过程的机制和能量特性
摘要 研究表明,链式反应过程的特点主要取决于初始试剂的大部分内能转化为原子和自由基的自由价能这一事实。这就导致了活性粒子的高浓度,它们以更高的速率与初始试剂发生反应,产生强烈的自热,从而进一步加速了过程。值得注意的是,如果不考虑反应的链式性质,就无法解释加热时的点火现象,因为只有分子试剂反应的高活化能排除了加热过程中速率的增加。考虑到燃烧反应的链式性质,就有可能解释加热时的点火现象,并发展出这一现象的理论。对气体燃烧的最重要特征做出了解释:反应链的长度决定了链式机制在燃烧中的作用,以及动力学对温度的依赖性。通过动力学和光谱学实验证实了第三可燃极限问题的解决方案,并获得了火焰中存在 HO2 自由基的证据,以及它们在反应链的异质发展和一般燃烧中的积极作用。实验证明,在描述燃烧时,可以用有效的动力学参数代替扩散微分方程的解法。
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来源期刊
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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