Methane oxidation;
Noble metals;
Platinum/alumina;
Palladium;
Turnover frequency (TOF);
Particle size effect;
In situ XPS;
RAY PHOTOELECTRON-SPECTROSCOPY;
PD/AL2O3;
CATALYSTS;
METHANE OXIDATION;
COMBUSTION;
BEHAVIOR;
D O I:
10.1007/s11244-013-9971-y
中图分类号:
O69 [应用化学];
学科分类号:
081704 ;
摘要:
Intrinsic catalytic activities (TOF values) in CH4 complete oxidation under lean conditions were estimated as a function of Pt and Pd particle sizes (d(m)) for two series of Pt/Al2O3 and Pd/Al2O3 catalysts. Comparison of TOF similar to f(d(m)) relationships revealed significant difference between Pt and Pd catalysts. For Pt catalyst TOF showed tendency to increase by 2-3 times with increasing particle size from 1 to ca 3 nm and remained constant, when Pt particles became larger than 3 nm. On the other hand, for Pd catalyst TOF increased almost linearly when particle size grew from 1 to 20 nm. These different tendencies were attributed to the different mechanisms of CH4 oxidation over Pt and Pd catalysts: Langmuir-Hinshelwood and Mars-Van Krevelen respectively.