Palladium is a very good catalyst for the combustion of methane. Supported palladium catalysts display an unusual behavior when they are first brought on stream under combustion conditions. The activity of the catalyst slowly increases over time at reaction conditions. This project examined this phenomenon for catalysts supported on silica. It was found that when the catalysts were prepared using a chloride precursor, there is residual chlorine left on the catalyst. When the catalyst is exposed to reaction conditions, it remains inactive until this chlorine is removed. Additional evidence was obtained suggesting that a palladium silicide might form during catalyst reduction and be related to the activity change over time.

“The Role of Chlorine in Induction Periods During the Oxidation of Methane over Pd/SiO₂,” S. S. Peri and C. R. F. Lund, J. Catal. 152, 410 (1995). [more info]

“Kinetic Changes During the Activation of Pd Methane Oxidation Catalysts.” C. R. F. Lund, S. S. Peri and S. Harou-Kouka, Preprints of Papers, Division of Petroleum Chemisry, ACS 42, 173, 1997.

“The Activation of Pd Catalysts during Oxidation of Methane,” Workshop on Advances in Homogeneous and Heterogeneous Catalysis and Surface Science, June 1996, Nanjing, China.

“Effect of Preparation and Pretreatment Methods on the Activity of Pd/SiO₂ in the Oxidation of Methane,” Annual AIChE Meeting, San Francisco, November 1994.

“Carburization of Pd During Catalytic Oxidation of Methane,” 1994 Gordon Conference on Catalysis, Colby-Sawyer College, NH, June 27 & 28 1994.

“Effect of Preparation and Pretreatment on the Activity of Pd/SiO₂ in the Oxidative Conversion of Methane,” SUNY-Buffalo, Chemical Engineering Department Seminar, April, 1994.

“Methane Oxidation over Palladium and Palladium-Copper Supported on Silica,” Annual AIChE Meeting, Miami Beach, November 1992.

Saley Harou-Kouka, “Microkinetic Modeling of Methane Oxidation on Silica Supported Palladium at Medium Temperature,” PhD Dissertation, University at Buffalo, SUNY, Dept. of Chemical Engineering (1999). [more info]

Sarveswara Sastry Peri, “Kinetics of Methane Oxidation on Supported Palladium Catalyst Systems,” PhD Dissertation, University at Buffalo, SUNY, Dept. of Chemical Engineering (1995). [more info]

Jane M. Lamanna, “Activation Behavior of a Silica-Supported Palladium Catalyst During Methane Oxidation,” M. S. Thesis, University at Buffalo, SUNY, Dept. of Chemical Engineering (1996). [more info]