原创力文档霍林河褐煤热解甲烷生成反应类型及动力学的热重-质谱实验与量子化学计算 Reaction Types and Kinetics of Methane Generation from Huolinhe Lignite Pyrolysis by TGMS Experiment and Quantum Chemical Calculations.pdfVIP
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物理化学学报(Wuli Huaxue Xuebao)
June A cta Phys. Chim. Sin., 2009, 25(6) ：1117-1124 1117
[Article]
霍林河褐煤热解甲烷生成反应类型及动力学的热重质谱
实验与量子化学计算
凡桂* 贾建波
(太原理工大学地球科学与工程系, 煤科学与技术教育部及山西省重点实验室, 太原 030024)
摘要： 应用开放体系的热重质谱联用技术(TG/MS)对未成熟的霍林河褐煤(镜质组最大反射率RO00 为0.33%)进
max
行了热解模拟, 获得了甲烷的在线析出速率曲线. 曲线拟合结果表明, 甲烷生成速率曲线可以分解为5 个峰, 结合
化学动力学分析, 发现低温阶段甲烷的峰为吸附甲烷析出峰, 其余四个峰为热解甲烷的生成峰, 代表四类不同的
化学反应. 将煤的结构特征及量子化学的理论计算相结合, 认为甲烷的生成包括4 类反应, 类型1 为与氧等杂原
子相连的脂碳断裂; 类型2 包含了两种反应, 一种是短链脂肪烃类官能团 位断裂, 另一种是所形成的长链脂肪
烃类物质二次裂解; 类型3 是与芳核直接相连的甲基热解脱落; 类型4 为存在于煤结构中脂肪类物质的芳香化.
关键词： 甲烷; 生成动力学; 煤结构; 量子化学计算; 霍林河褐煤
中图分类号： O641; O643
Reaction Types and Kinetics of Methane Generation from Huolinhe
Lignite Pyrolysis by TG/MS Experiment and Quantum Chemical
Calculations
ZENG Fan Gui* JIA Jian Bo
(Key Laboratory of Coal Science Technology, Ministry of Education Shanxi Province, Dep artment of Earth Science
Engineering, Taiyuan University of Technology, Taiyuan 030024, P. R. China)
Abstract ： Open system pyrolysis modeling of immature Huolinhe lignite (vitrinite reflectivity, RO00 of 0.33%) was
max
carried out and an on line curve for the methane generation rate was obta
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