Kinetic Modeling of the Metal/Support Interaction for CH4 Reaction over Oxidized Pd/Al2O3
Kinetic Modeling of the Metal/Support Interaction for CH4 Reaction over Oxidized Pd/Al2O3
复制标题
氧化 Pd/Al2O3 上 CH4 反应的金属/载体相互作用的动力学模型
DOI：
10.1007/s11244-018-1125-9
复制
发表时间：
2018
影响因子：
3.6
通讯作者：
P. Granger
中科院分区：
文献类型：
--
作者：
F. Dhainaut;P. Granger
本文研究了Pd/Al_2O_3催化剂上甲烷的解离动力学。用TAP反应器研究了CH 4在新鲜和老化的氧化型催化剂上的吸附和转化。在稳定的表面上进行了单次CH 4脉冲TAP实验。实验进行了讨论，在选定的机制，涉及CH 4分解成CO2考虑到金属活性位点和支持之间的相互作用。TAP实验的氧化催化剂确认参与的金属/载体界面，溢出效应。优化的动力学参数验证这种相互作用的OH物种吸附在钯网站与氧化铝，实验和计算的出口气体组成之间的相对较好的协议。新鲜和老化的催化剂都遵循所选择的机制，在400 °C下具有相同的动力学常数，只有催化表面积的改变解释了活性的损失。
This paper deals with the kinetics of CH4dissociation on model Pd/Al2O3catalysts. The adsorption and conversion of CH4over oxidized catalysts, fresh or aged, were studied with a temporal analysis of products (TAP) reactor. Single CH4pulse TAP experiments were performed on a stabilized surface. The experiments are discussed in the light of a selected mechanism involving CH4decomposition into CO2taking into account an interaction between the metallic active sites and the support. TAP experiments over the oxidized catalysts confirm the involvement of the metal/support interface, with a spill-over effect. Optimized kinetics parameters validate this interaction of OH species adsorbed on Pd sites with alumina, showing a relatively good agreement between experimental and calculated outlet gas composition. Both fresh and aged catalysts follow the chosen mechanism with the same kinetic constants at 400 °C only an alteration of the catalytic surface areas explain the loss of activity.