光学精密工程2026，Vol.34Issue(6)：861-873,13.DOI:10.37188/OPE.20263406.0861
结合TG-TDLAS与ReaxFF MD的烟煤热解CH₄生成机理研究
Study on the mechanism of CH₄ formation from bituminous coal pyrolysis combining TG-TDLAS and ReaxFF molecular dynamic
摘要
Abstract
To elucidate the mechanism of methane(CH₄)formation during bituminous coal pyrolysis at the atomic scale,addressing the limitations of traditional experimental methods in capturing reaction pre⁃cursors and microscopic pathways,this study employed a combined approach of thermogravimetric-tune⁃able diode laser absorption spectroscopy(TG-TDLAS)experiments and reaction molecular dynamics sim⁃ulations(ReaxFF MD).First,TG-TDLAS experiments were conducted to obtain the macroscopic tem⁃perature dependence and kinetic behavior of CH₄ generation.Second,based on elemental analysis,infra⁃red spectroscopy,and ¹³C NMR characterization of bituminous coal samples,a molecular model(C₃₀₉H₂₀₃N₃O₁₈)was constructed.ReaxFF MD simulations analyzed the dynamic reaction processes of CH₃ radical cleavage,hydrogen migration,and CH₄ formation at different temperatures.Results indicate that experi⁃mentally measured CH₄ production peaks around 600 ℃ within the 450–750 ℃ range.Simulations reveal the microscopic mechanism:side-chain CH₃ fragments at approximately 1 100 K to form radicals,which subsequently convert to CH₄ by abstracting adjacent hydrogen atoms,peaking at 2 500 K.Both measure⁃ments show high consistency in production trends.The conclusion asserts that this method systematically elucidates,from both macroscopic and microscopic perspectives,that CH₄ generation stems from the equi⁃librium process between precursor fragmentation and hydrogen abstraction.It validates the unique advan⁃tage of ReaxFF MD in revealing the behavior of intermediates within the complex reaction network of coal pyrolysis,providing a theoretical basis for understanding coal spontaneous combustion,pyrolysis path⁃ways,and enhancing energy conversion efficiency.关键词
ReaxFF MD/热解/煤分子模型/CH4Key words
ReaxFF MD/pyrolysis/coal molecule model/CH4分类
数理科学引用本文复制引用
王庚乾,张君瑞,王远洋,李光跃,田亚莉,和小虎,邱选兵,李传亮,梁五洲,姚凯..结合TG-TDLAS与ReaxFF MD的烟煤热解CH₄生成机理研究[J].光学精密工程,2026,34(6):861-873,13.基金项目
国家自然科学基金(No.52076145,No.62475182) （No.52076145,No.62475182）
山西省重点研发计划(No.202402150301012) （No.202402150301012）
山西省基础研究计划(No.202303021221147) （No.202303021221147）
山西省科技创新人才团队专项资助(No.202304051001034) （No.202304051001034）
中央引导地方科技发展资金项目(No.YDZJSX2025C026) （No.YDZJSX2025C026）
太原科技大学科研启动基金(No.20222121,No.20232033) （No.20222121,No.20232033）
量子光学与光量子器件国家重点实验室开放课题(No.KF202305) （No.KF202305）
