Methane Combustion over Pd/Al<sub>2</sub>O<sub>3</sub> Catalysts in the Presence of Water: Effects of Pd Particle Size and Alumina Crystalline Phase
Kazumasa Murata, Junya Ohyama, Yuta Yamamoto, Shigeo Arai, Atsushi Satsuma
Abstract
The effects of the Pd particle size and the Al2O3 crystalline phase of Pd/Al2O3 catalysts on the CH4 combustion in the presence of H2O were investigated. According to X-ray absorption fine structure (XAFS) measurements, it was revealed that, during the CH4 combustion, the Pd nanoparticles existed on the Al2O3 support as a PdO phase, while the crystallinity of PdO depended on the Pd particle size. On the basis of X-ray diffraction (XRD), amorphous PdO particles with a size of <7 nm exhibited low activity for CH4 combustion. In contrast, as the Pd particle size increased, larger crystalline PdO particles (>7 nm) were formed, which were highly active for CH4 combustion. Comparing the effects of the different Al2O3 crystalline phases, Pd/α-Al2O3 was proved to be more resistant to deactivation by H2O than Pd/γ-Al2O3 and Pd/θ-Al2O3. Moreover, according to H2O temperature-programmed desorption (TPD) and infrared (IR) measurements, since α-Al2O3 was relatively hydrophobic compared to γ-Al2O3 and θ-Al2O3, a faster and reversible adsorption/desorption of OH/H2O species was achieved, while the H2O poisoning on PdO species in the vicinity was limited.