Report

Exceptional Activity for Methane Combustion over Modular Pd@CeO2 Subunits on Functionalized Al2O3

Science  10 Aug 2012:
Vol. 337, Issue 6095, pp. 713-717
DOI: 10.1126/science.1222887

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Addressing a Burning Issue

Complete combustion of methane is required in order to avoid the unproductive emission of this greenhouse gas into the atmosphere. Palladium catalysts can help to promote complete combustion, but high-temperature operating conditions also promote aggregation of catalyst particles (“sintering”) that lowers their surface area and overall activity. Cargnello et al. (p. 713; see the Perspective by Farrauto) report that cerium oxide–coated Pd catalyst particles could be fully dispersed on an alumina surface prepared with a hydrophobic coating. This treatment resisted Pd sintering up to temperatures of 800°C, and also enabled complete combustion of methane to occur at temperatures as low as 400°C.

Abstract

There is a critical need for improved methane-oxidation catalysts to both reduce emissions of methane, a greenhouse gas, and improve the performance of gas turbines. However, materials that are currently available either have low activity below 400°C or are unstable at higher temperatures. Here, we describe a supramolecular approach in which single units composed of a palladium (Pd) core and a ceria (CeO2) shell are preorganized in solution and then homogeneously deposited onto a modified hydrophobic alumina. Electron microscopy and other structural methods revealed that the Pd cores remained isolated even after heating the catalyst to 850°C. Enhanced metal-support interactions led to exceptionally high methane oxidation, with complete conversion below 400°C and outstanding thermal stability under demanding conditions.

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