激发态在AC等离子体辅助甲烷裂解及低温氧化过程中的作用机理研究.docxVIP

中国工程热物理学会 燃烧学 学术会议论文 编号：184031 激发态在AC等离子体辅助甲烷裂解及低温氧化过程中的作用机理研究 孙进桃，陈琪*，许京 机械与电子控制工程学院，北京交通大学，北京100044 Tel Email:qchen@ 摘 要 本文采用实验测量和数值模拟结合的方法，对AC放电下CH4/O2/He混合气中激发态对甲烷裂解和低温氧化的动力学贡献进行研究。基于HP-Mech，增加反应物的放电机理以及激发态参与的化学反应及其驰豫反应，建立CH4低温氧化机理。采用化学反应动力学求解器CHEMKIN中的两段式Plasma-PSR模型模拟放电过程及化学反应过程。该动力学模型能较好地预测反应物的消耗和主要产物的生成，反应路径分析表明激发态物质CH4(v), O2(v), O2(a1Δg)等通过链式反应CH4(v)+OH→CH3+H2O, O2(v)+H→OH+O, O2(a1Δg)+H→O+OH促进活性自由基和产物的生成。 关键词 交流放电激励；激发态；甲烷裂解和氧化；路径通量分析 Kinetic effects of excited states on AC plasma assisted-methane pyrolysis and oxidation Jintao Sun, Qi Chen*, Jing Xu School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing, 100044 Tel Email:qchen@ Abstract: Methane pyrolysis and oxidation by excited states in AC discharges was studied in CH4/O2/He mixtures by methods of experimental measurements and numerical simulations. The comprehensive HP-Mech, modeled the rate coefficients of elementary reactions. Other reactions were integrated for describing the evolution of a plasma reforming system, including electron impact reactions, electron-ion recombination reactions and reactions involving excited species. Steady state kinetic results showed a liner increase in methane conversion with the increase of plasma power, suggesting the strong dependence of non-equilibrium excitation process on RF discharge parameters. Numerical comparisons with steady state measurements showed a significant agreement. Analysis of reaction pathways indicates that vibrational species CH4(v), O2(v), O2(a1Δg) enhances chain propagating reactions CH4(v)+OH→CH3+H2O, O2(v)+H→OH+O, O2(a1Δg)+H→OH+O, thus stimulating the production of active radicals and final products. This work provided a fundamental understanding for the roles of excited species in low temperature oxidation of methane. Key words: AC discharge; ex