The natural abundance of copper and cuprous oxide (Cu2O), its tunable electronic properties and its optimal catalytic performance for reactions from CO oxidation, water-gas shift (WGS) to methanol synthesis have made it a prime target for catalytic research. While the controlled synthesis of nanoscale cuprous oxide particles is being actively pursued to optimize its properties, the Achilles heel of Cu2O catalysts has been its deactivation by complete oxidation to CuO or reduction to Cu, in both cases losing the critically active catalytic Cu+ centers. The oxidation of CO (CO+1/2O2=CO2) is the archetypal heterogeneous catalytic reaction, playing a central role in the advancement of fundamental studies, the control of automobile emissions and industrial oxidation reactions. Copper-based catalysts were the first reported to run CO oxidation at room temperature, but their lack of stability at the elevated reaction temperatures used on automobile catalytic converters, in particular the loss of the most reactive Cu+ cations, leads to their deactivation. Using a combined experimental and theoretical approach, we show how the incorporation of Ti cations in a Cu2O film leads to the formation of a stable mixed-metal oxide, with a Cu+ terminated surface highly active for CO oxidation.[1] The oxidation of CO during the WGS reaction (CO+H2O=CO2+H2) occurs in this case under an overall reducing environment. We show how the formation of a multifunctional metal-oxide interface with ceria nanoparticles allows the stabilization of critical intermediates for an efficient associative reaction mechanism.[2] We will finally show that a similar metal-oxide interface can help to activate copper for the thermal reduction of CO2.[1] �Importance of the Metal-Oxide Interface in Catalysis: In-situ Studies by Ambient-Pressure XPS of the Water-Gas Shift Reaction� K Mudiyanselage, SD Senanayake, L Feria, S Kundu, AE Baber, J Graciani, AB Vidal, S Agnoli, J Evans, R Chang, S Axnanda, Z Liu, JF Sanz, P Liu, JA Rodriguez, DJ StacchiolaAngew. Chem. Int. Ed. 52 , 5101�5105 (2013)[2] �Stabilization of catalytically active Cu+ surface sites on titanium-copper mixed oxide films� AE Baber, X Yang, HY Kim, K Mudiyanselage, M Soldemo, J Weissenrieder, SD Senanayake, A Al-Mahboob, JT Sadowski, J Evans, JA Rodriguez, P Liu, FM Hoffmann, JG Chen, DJ StacchiolaAngew. Chem. Int. Ed. (in Press)

Tuning the activity and stability of copper based catalysts with reducible oxides

248th National Meeting (2014)

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