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Open Access Perovskite-supported Palladium for Methane Oxidation – Structure–Activity Relationships

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Palladium is the precious metal of choice for methane oxidation and perovskite-type oxides offer the possibility to stabilize it as PdO, considered crucial for catalytic activity. Pd can adopt different oxidation and coordination states when associated with perovskite-type oxides. Here, we review our work on the effect of perovskite composition on the oxidation and coordination states of Pd and its influence on catalytic activity for methane oxidation in the case of typical Mn, Fe and Co perovskite-based oxidation catalysts. Especially X-ray absorption near edge structure (XANES) spectroscopy is shown to be crucial to fingerprint the different coordination states of Pd. Pd substitutes Fe and Co in the octahedral sites but without modifying catalytic activity with respect to the Pd-free perovskite. On LaMnO3 palladium is predominantly exposed at the surface thus bestowing catalytic activity for methane oxidation. However, the occupancy of B-cation sites of the perovskite structure by Pd can be exploited to cyclically activate Pd and to protect it from particle growth. This is explicitly demonstrated for La(Fe, Pd)O3, where catalytic activity for methane oxidation is enhanced under oscillating redox conditions at 500 °C, therefore paving the way to the practical application in three-way catalysts for stoichiometric natural gas engines.

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Keywords: AUTOMOTIVE CATALYSIS; METHANE; OCTAHEDRAL COORDINATION; PALLADIUM; PEROVSKITE

Document Type: Research Article

Affiliations: 1: Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, Ueberlandstrasse 129, CH-8600 Dübendorf, Switzerland 2: Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Solid State Chemistry and Catalysis, Ueberlandstrasse 129, CH-8600 Dübendorf, Switzerland. [email protected]

Publication date: September 1, 2012

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  • International Journal for Chemistry and Official Membership Journal of the Swiss Chemical Society (SCS) and its Divisions

    CHIMIA, a scientific journal for chemistry in the broadest sense, is published 10 times a year and covers the interests of a wide and diverse readership. Contributions from all fields of chemistry and related areas are considered for publication in the form of Review Articles and Notes. A characteristic feature of CHIMIA are the thematic issues, each devoted to an area of great current significance.

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