摘要
本文采用实验测量和数值模拟结合的方法,对NSD等离子体-催化剂协同重整CH_(4)/CO_(2)过程中的协同效应以及积碳动力学进行研究。构建了包含中性分子、自由基、振动激发态、电子激发态、带电粒子、表面吸附态等物质在内的详细动力学机理。采用ZDPlasKin-CHEMKIN耦合的方法迭代求解等离子体放电过程、气相反应动力学及表面反应动力学在内的详细动力学机理。在300~700 K的温度范围内,该动力学模型能较好地预测反应物的消耗和产物的生成,路径通量分析表明CH_(3)在催化剂表面上的直接吸附反应以及CH_(4)振动激发态分子的吸附态CH_(4)(vs)在催化剂表面上的解离吸附均可促进吸附态CH_(3)(s)的生成。积碳动力学研究表明催化剂上的积碳主要来源于吸附态CH(s)的脱氢反应CH(s)+Ni(s)→C(s)+H(s)。
The present work investigates the synergistic effects and coking kinetics of catalytic CH_(4)/CO_(2) reforming activated by a nanosecond pulsed discharge(NSD)plasma experimentally and numerically.A detailed plasma catalysis kinetic mechanism consisting of neutral molecules,radicals,excited species,ions,and surface adsorbed species is developed and studied.A zero-dimensional model incorporating the plasma kinetics solver ZDPlasKin and the combustion chemical kinetics solver CHEMKIN is used to calculate the plasma kinetics,gas-phase kinetics and surface kinetics.In the temperature range of 300~700 K,the consumption of reactants and the formation of products are well captured by the kinetic model and show a reasonable agreement.The path flux shows that the direct adsorption of CH_(3) and the dissociative adsorption of adsorbed CH_(4)(vs)on the catalyst surface can promote the formation of adsorbed CH_(3)(s).Coking kinetics investigation indicates that the carbon deposition on the catalyst mainly comes from the dehydrogenation reaction of adsorbed CH(s):CH(s)+Ni(s)→C(s)+H(s).
作者
孙进桃
赵旭腾
陈琪
林赫
SUN Jintao;ZHAO Xuteng;CHEN Qi;LIN He(School of Mechanical,Electronic and Control Engineering,Beijing Jiaotong University,Beijing 100044,China;The Institute of Advanced Energy and Powertrain Technology,Shanghai Jiao Tong University,Shanghai 200240,China)
出处
《工程热物理学报》
EI
CAS
CSCD
北大核心
2023年第5期1428-1437,共10页
Journal of Engineering Thermophysics
基金
国家自然科学基金资助项目(No.21975018)。
