Kinetic Analysis of the Generation of Active Sites During the Low-Temperature Pyrolysis of Coal

热解 活化能 分解 化学 热重分析 等温过程 动力学 反应级数 热分解 动能 反应速率 化学动力学 分析化学(期刊) 热力学 反应速率常数 物理化学 催化作用 有机化学 物理 量子力学
作者
Jingjuan Geng,Jinhu Li,Yongliang Yang,Zenghua Li,Wei Peng
出处
期刊:Combustion Science and Technology [Taylor & Francis]
卷期号:196 (3): 352-370 被引量:2
标识
DOI:10.1080/00102202.2022.2079377
摘要

Decomposition of oxygen-containing functional groups simultaneously produces CO and CO2, accompanied by the generation of active sites. Two different methods were applied in the study to speculate the kinetics of gas generation and the formation of active sites in coal pyrolysis. The evolution of CO and CO2 gas generation during isothermal pyrolysis under different temperatures was first analyzed, and the generation of CO and CO2 in the pyrolysis process was divided into three stages: the rapid decline stage, slow decline stage, and stabilization stage. In the early stage of the pyrolysis reaction, functional groups exhibited a rapid decomposition rate and a high conversion rate (a), which rapidly decreased the gas concentrations. With increasing pyrolysis time, the decomposition of functional groups declined with a low conversion rate (a) and showed a steady reaction rate in the later stage. On this basis, a method to calculate the activation energy during pyrolysis based on the data of gases generated in a steady period with a continuous cooling temperature was proposed. Activation energies of 70.12–148.39 kJ/mol for the CO formation and 64.47–127.38 kJ/mol for the CO2 formation were obtained from four different coals. In addition, a thermogravimetric analyzer was used to explore the apparent activation energies in the decomposition process via Coats-Redfern (C-R) method; activation energies of 39.33–126.65 kJ/mol and pre-exponential factors of 1.31–5.15E+08 s−1 were obtained for different coals. The results revealed that the CO had a greater generation activation energy than CO2, and a higher metamorphism degree implies a higher decomposition activation energy, which indicates that the decomposition of carboxyl groups and low-rank coals result in higher active sites.
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