Abstract
Elaboration of Pd-supported catalysts for catalytic combustion is, nowadays, considered as an imperative task to reduce the emissions of methane. This study provides new insight into the method of deposition, chemical state of Pd and oxygen storage capability of transition metal ions and their effects on the catalytic reactivity of supported catalysts for the combustion of methane. The catalyst with nominal composition La(Co0.8Ni0.1Fe0.1)0.85Pd0.15O3 was supported on SiO2-modified/γ-alumina using two synthetic procedures: (i) aerosol assisted chemical vapor deposition (U-AACVD) and (ii) wet impregnation (Imp). A comparative analysis shows that a higher catalytic activity is established for supported catalyst obtained by wet impregnation, where the PdO-like phase is well dispersed and the transition metal ions display a high oxygen storage capability. The reaction pathway over both catalysts proceeds most probably through Mars–van Krevelen mechanism. The supported catalysts are thermally stable when they are aged at 505 °C for 120 h in air containing 1.2 vol.% water vapor. Furthermore, the experimentally obtained data on La(Co0.8Ni0.1Fe0.1)0.85Pd0.15O3—based catalyst, supported on monolithic substrate VDM®Aluchrom Y Hf are simulated by using a two-dimensional heterogeneous model for monolithic reactor in order to predict the performance of an industrial catalytic reactor for abatement of methane emissions.
Highlights
IntroductionAt present time there is an increased interest in the application of methane (as the main component of natural gas) as a fuel in the internal combustion engines
In comparison with Pd-LMO/Imp, the Pd-LMO/U-aerosol assisted chemical vapor deposition (AACVD) sample contains relatively higher amounts of the perovskite phase and it undergoes a significant change after the catalytic reaction due to the extraction of Pd from the perovskite structure during the catalytic reaction
The impregnation of SiO2 -modified/γ-alumina support with citrate solutions of La, Co, Ni, Fe and Pd leads to a deposition of an intimate mixture of well dispersed PdO-like phase, transition metal oxides and Pd-containing perovskite on the support surface, while the aerosol assisted chemical vapor deposition of the same citrate solution yields a Pd-containing perovskite phase as the main product
Summary
At present time there is an increased interest in the application of methane (as the main component of natural gas) as a fuel in the internal combustion engines. Bordelanne and co-workers [3] reported that GHG emissions from vehicles on compressed natural gas (CNG) fuel may produce significantly lower emissions than of gasoline vehicles and in case of hybrid CNG vehicles the reduction of 51% can be reached. In the case of the Toyota Prius CNG Hybrid prototype fuelled by biomethane produced from waste (in comparison to a gasoline vehicle), the emissions are lowered by 87% [3]. The use of biomethane can lead to reduction of GHG emissions below the minimum specified by the European Directive on the Promotion of Renewable Energy Sources (2009/28/EC)
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