介质阻挡放电辅助甲烷蒸汽重整的动力学分析

Kinetic analysis of methane steam reforming assisted by dielectric barrier discharge

为了发展可用于等离子辅助甲烷蒸汽重整的详细反应机理,采用数值模拟和实验研究相结合的方法,系统分析了停留时间、水蒸气/甲烷摩尔比及其反应温度对甲烷转化率和产物产量的影响规律。结合一组实验数据,发展和评估了等离子体辅助甲烷蒸汽重整的详细反应动力学机理。与实验结果对比表明:该动力学机理可以准确预测甲烷转化率及其各产物产量的变化趋势。路径流分析表明CH3基再结合是CH4转化为CO的主要限制步,O基是影响CO生成的关键组分。并列式协同催化实验中有效碳回收率达到100%,该结果初步证实了路径流分析结果的正确性。所做研究明确了等离子体催化甲烷重整的特性,为非平衡等离子体与催化剂协同催化甲烷蒸汽重整的机理研究奠定了基础。

To develop a detailed reaction mechanism for plasma-assisted methane steam reforming,a comprehensive numerical and experimental study of the effect laws on methane conversion and products yield was performed at different resident time,steam to methane molar ratio and reaction temperature. Combined with a group of experimental results,a detailed kinetic reaction mechanism for plasma-assisted methane steam reforming was developed and evaluated. A set of comparisons with experimental results showed the reaction mechanism could accurately predict methane conversion and the change trend of products yield. The path flux analysis showed that CH3 recombination was the limiting reaction for CO production,while O was the critical species for CO production. The validity of path flux analysis result was preliminarily verified by the experiment of plasma catalytic hybrid reaction,where the effective carbon recovery rate was up to 100%. The proposed research ascertains the characters of methane steam reforming by Dielectric Barrier Discharges（ DBD）,and lays the foundation for the research of the non-equilibrium plasma and catalyst hybrid reaction mechanism for methane steam reforming.