无机材料学报 ›› 2024, Vol. 39 ›› Issue (11): 1235-1244.DOI: 10.15541/jim20240158 CSTR: 32189.14.10.15541/jim20240158

• 研究论文 • 上一篇    下一篇

CH4+C2H5OH+Ar体系热解的气相动力学研究

马永杰1(), 刘永胜1, 关康2(), 曾庆丰3()   

  1. 1.西北工业大学 超高温结构复合材料重点实验室, 西安 710072
    2.华南理工大学 材料科学与工程学院, 广州 510640
    3.天目山实验室 高性能航空材料与先进制造中心, 杭州 311115
  • 收稿日期:2024-04-01 修回日期:2024-06-21 出版日期:2024-11-20 网络出版日期:2024-06-24
  • 通讯作者: 关 康, 副教授. E-mail: mskguan@scut.edu.cn;
    曾庆丰, 研究员. E-mail: bht0045@tmslab.cn
  • 作者简介:马永杰(1999-), 男, 硕士研究生. E-mail: mayongjie@mail.nwpu.edu.cn
  • 基金资助:
    浙江省重点研发计划(2024SSYS0085);国家自然科学基金(51702100);国家自然科学基金(51972268);广东省基础与应用基础研究基金(2023A1515012156);广东省基础与应用基础研究基金(2024A1515011656);中央高校基本科研业务费专项资金(2022ZYGXZR026)

Gas-phase Kinetic Study of Pyrolysis in the System of CH4+C2H5OH+Ar

MA Yongjie1(), LIU Yongsheng1, GUAN Kang2(), ZENG Qingfeng3()   

  1. 1. Science and Technology on Thermostructural Composite Materials Laboratory, Northwestern Polytechnical University, Xi'an 710072, China
    2. School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China
    3. High Performance Aviation Materials and Advanced Manufacturing Center, Tianmushan Laboratory, Hangzhou 311115, China
  • Received:2024-04-01 Revised:2024-06-21 Published:2024-11-20 Online:2024-06-24
  • Contact: GUAN Kang, associate professor. E-mail: mskguan@scut.edu.cn;
    ZENG Qingfeng, professor. E-mail: bht0045@tmslab.cn
  • About author:MA Yongjie (1999-), male, Master candidate. E-mail: mayongjie@mail.nwpu.edu.cn
  • Supported by:
    Key R&D Program of Zhejiang(2024SSYS0085);National Natural Science Foundation of China(51702100);National Natural Science Foundation of China(51972268);Guangdong Basic and Applied Basic Research Foundation(2023A1515012156);Guangdong Basic and Applied Basic Research Foundation(2024A1515011656);Fundamental Research Funds for the Central Universities(2022ZYGXZR026)

摘要:

通过化学气相渗透工艺, 利用以CH4和C2H5OH为前驱体制备碳/碳复合材料, 可以提高沉积速率且易得到高织构的热解炭。探究其反应机制可以更好地用于计算流体力学(CFD)研究。化学反应机制往往包含大量自由基和反应, 而以实验为主手动构建反应机制很容易遗漏重要物质和反应。本研究利用反应机制生成器(RMG)构建了CH4+C2H5OH+Ar体系详细的气相热解动力学机制, 其涵盖31种核心物质和214个核心反应, 预测了主要物质形成和消耗的趋势, 模拟结果与实验结果趋势相吻合。通过详细的动力学机制研究和反应物以及部分重要产物灵敏度分析, 识别了影响关键物质生成和消耗的反应。反应路径分析揭示了详细机制中不同物质之间的关系, 并确定了机制中的核心物质。在温度1373 K、压力10 kPa条件下, 依据灵敏度分析和路径分析的结果对详细机制进行了简化, 得到包含18种物质和44个反应的气相简化动力学机制。该简化机制在保留关键物质的同时显著提高了计算效率, 为进一步CFD研究和应用提供了更为便利的基础。

关键词: 碳/碳复合材料, 气相动力学, 机制分析, 机制简化

Abstract:

Preparation of carbon-carbon composites through the chemical vapor infiltration (CVI) process, utilizing CH4 and C2H5OH as precursors, can effectively improve the deposition rate and produce highly structured pyrolytic carbon. Understanding the reaction mechanism is essential for computational fluid dynamics (CFD) studies. Chemical reaction mechanisms typically involve numerous free radicals and reactions, and manually constructing such mechanisms based on experimental data alone risks omitting critical species and reactions. Hence, in this research, a thorough gas-phase pyrolysis kinetic mechanism for the CH4+C2H5OH+Ar system was developed using the reaction mechanism generator (RMG). This mechanism included 31 core species and 214 core reactions, accurately predicting the evolution of major species' formation and consumption. The simulation results were consistent with experimental observations. Through a detailed analysis of the kinetics and sensitivity of reactants and critical products, reactions influencing the formation and consumption of crucial species were identified. Reaction pathway analysis further clarified relationships among different species, identifying core species within the mechanism. By simplifying the detailed mechanism based on sensitivity and rection pathway analysis at 1373 K and 10 kPa, a gas-phase kinetic mechanism was derived, composed of 18 species and 44 reactions. This streamlined model substantially boosts computational efficiency while retaining key species, providing a more convenient foundation for further CFD studies and applications.

Key words: carbon/carbon composite, gas-phase dynamic, mechanism analysis, mechanism simplification

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