Metal-Support Interactions and C1 Chemistry: Transforming Pt-CeO2into a Highly Active and Stable Catalyst for the Conversion of Carbon Dioxide and Methane

• Autores: Zhang, Feng; Gutiérrez, Ramón A.; Lustemberg, Pablo German; Liu, Zongyuan; Rui, Ning; Wu, Tianpin; Ramírez, Pedro J.; Xu, Wenqian; Idriss, Hicham; Ganduglia Pirovano, M. Verónica; Senanayake, Sanjaya D.; Rodriguez, José A.
• Año de publicación: 2021
• Idioma: inglés
• Tipo de recurso: artículo
• Materia: C1 CHEMISTRY; CH4CONVERSION; CO2CONVERSION; METAL-SUPPORT INTERACTIONS; METHANE DRY REFORMING; PLATINUM
• Institución: Consejo Nacional de Investigaciones Científicas y Técnicas

There is an ongoing search for materials which can accomplish the activation of two dangerous greenhouse gases like carbon dioxide and methane. In the area of C1 chemistry, the reaction between CO2 and CH4 to produce syngas (CO/H2), known as methane dry reforming (MDR), is attracting a lot of interest due to its green nature. On Pt(111), high temperatures must be used to activate the reactants, leading to a substantial deposition of carbon which makes this metal surface useless for the MDR process. In this study, we show that strong metal-support interactions present in Pt/CeO2(111) and Pt/CeO2 powders lead to systems which can bind CO2 and CH4 well at room temperature and are excellent and stable catalysts for the MDR process at moderate temperature (500 °C). The behavior of these systems was studied using a combination of in situ/operando methods (AP-XPS, XRD, and XAFS) which pointed to an active Pt-CeO2-x interface. In this interface, the oxide is far from being a passive spectator. It modifies the chemical properties of Pt, facilitating improved methane dissociation, and is directly involved in the adsorption and dissociation of CO2 making the MDR catalytic cycle possible. A comparison of the benefits gained by the use of an effective metal-oxide interface and those obtained by plain bimetallic bonding indicates that the former is much more important when optimizing the C1 chemistry associated with CO2 and CH4 conversion. The presence of elements with a different chemical nature at the metal-oxide interface opens the possibility for truly cooperative interactions in the activation of C-O and C-H bonds.
Fil: Zhang, Feng. State University of New York. Stony Brook University; Estados Unidos
Fil: Gutiérrez, Ramón A.. Universidad Central de Venezuela; Venezuela
Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina. Consejo Superior de Investigaciones Científicas; España
Fil: Liu, Zongyuan. Brookhaven National Laboratory; Estados Unidos
Fil: Rui, Ning. Brookhaven National Laboratory; Estados Unidos
Fil: Wu, Tianpin. Argonne National Laboratory; Estados Unidos
Fil: Ramírez, Pedro J.. Zoneca-cenex; México. Universidad Central de Venezuela; Venezuela
Fil: Xu, Wenqian. Argonne National Laboratory; Estados Unidos
Fil: Idriss, Hicham. King Abdullah University of Science and Technology; Arabia Saudita
Fil: Ganduglia Pirovano, M. Verónica. Consejo Superior de Investigaciones Científicas; España
Fil: Senanayake, Sanjaya D.. Brookhaven National Laboratory; Estados Unidos
Fil: Rodriguez, José A.. Brookhaven National Laboratory; Estados Unidos. State University of New York. Stony Brook University; Estados Unidos