Kinetics of methane combustion on model supported Pd/LaxMnO3 natural gas vehicle catalysts: Sensitivity of La-stoichiometry on the catalytic properties of Pd

被引:3
作者
Zheng, Yuanshuang [1 ]
Marinova, Maya [2 ]
Granger, Pascal [1 ]
机构
[1] Univ Lille, Univ Artois, UCCS Unite Catalyse & Chim Solide, CNRS,UMR 8181,ENSCL,Cent Lille, F-59000 Lille, France
[2] Univ Lille, Univ Artois, IMEC Inst Michel Eugene Chevreul, CNRS,INRAE,Cent Lille,FR 2638, F-59000 Lille, France
关键词
Methane combustion; Post-combustion catalysis; Palladium; Perovskite; Kinetics; COMPLETE OXIDATION; LAMNO3; PEROVSKITE; CH4; OXIDATION; PALLADIUM; NO; TEMPERATURE; REACTIVITY; ABATEMENT; OXYGEN; CO;
D O I
10.1016/j.cej.2023.146389
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The kinetics of the catalytic CH4/O-2 reaction has been studied on 1 wt% Pd/LaxMnO3 with x = 0.7, 1.0 and 1.3. Steady-state kinetic measurements have been performed in lean conditions at 400 degrees C on pre-reduced and on aged catalysts after exposure to wet atmosphere at 750 degrees C. A single site reaction mechanism occurs preferentially on Pd/La1.3MnO3 exhibiting a La-rich surface. In contrast a dual-site reaction mechanism, combining Pd and surface reactive oxygen species from the support, is preferentially involved on Pd-La0.7MnO3 characterized by a Mn-rich surface. Pd/LaMnO3 exhibits a mixed regime but subsequent deterioration of the Pd-LaxMnO3 interface during thermal aging leads to increasing contribution of the single site reaction mechanism. High surface Pd/Mn ratio and high concentration of Pd-n(+) with n > 2 can be considered as good descriptors to probe the efficacy of Pd/LaxMnO3 catalysts. Remarkably, the high thermal stability of the Pd-La0.7MnO3 interface, preserving the Pd dispersion on Pd/La0.7MnO3, leads to lower sensitivity to deactivation.
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页数:13
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