Total oxidation of methane over Pd/Al2O3at pressures from 1 to 10 atm
Journal article, 2020

The kinetics of total methane oxidation over a 0.15 wt% Pd/Al2O3 monolith catalyst has been measured during temperature programmed methane oxidation experiments at total pressures from 1 to 10 atm and compared with multiscale simulations. The methane conversion can be significantly enhanced by increasing the total pressure at temperatures above 350 °C, which is thanks to a longer residence time that dominates over decreased bulk gas diffusion rates and product inhibition. For the present catalyst, the external mass transfer impacts the methane conversion above 4 atm. With increasing total pressure, the observed methane reactions order decreases at 350 °C whereas it increases at 450 °C due to a more pronounced product inhibition at the lower temperatures. This is also reflected in the apparent activation energy, which increases with increasing total pressure. The multiscale simulations capture the general trends of the experimental results but overestimate the methane conversion at higher temperatures and total pressures. The overestimated activity indicates of an overestimated number of active sites and/or an underestimated external mass transfer resistance.

Author

Carl-Robert Florén

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Polymer Technology

Cansunur Demirci

Istituto Italiano di Tecnologia

University of Genoa

Per-Anders Carlsson

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Per-Anders Carlsson Group

Derek Creaser

Chalmers, Chemistry and Chemical Engineering, Chemical Technology, Chemical Process and Reaction Engineering

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Polymer Technology

Catalysis Science and Technology

2044-4753 (ISSN) 2044-4761 (eISSN)

Vol. 10 16 5480-5486

Subject Categories

Chemical Process Engineering

Other Chemical Engineering

Metallurgy and Metallic Materials

DOI

10.1039/d0cy00813c

More information

Latest update

2/8/2021 4