Pt-based Catalysts in the Dry Reforming of Methane: Effect of Support and Metal Precursor on the Catalytic Stability
DOI:
https://doi.org/10.29356/jmcs.v65i1.1262Keywords:
Methane dry reforming, Pt/Ceria, metal-support interaction, catalytic stabilityAbstract
Abstract. Platinum catalysts (1.5 wt. %) supported over CeO2 and γ-Al2O3 were synthesized via wet impregnation using two different Pt precursors: H2PtCl6 and Pt(acac)2. Catalysts were tested in the dry reforming of methane (DRM) reaction at stoichiometric conditions (CH4/CO2 molar ratio of 1) with two approaches: as a function of temperature (400-800 °C) and as a function of time on-stream (800 °C / 24 h). Platinum supported over ceria catalysts showed better catalytic properties, especially in the stability tests, where deactivation was almost negligible. In contrast, alumina-supported catalysts stability was considerably lower due to the increased formation of carbon residues and the significant Pt particle sintering after reaction at 800 °C for 24 h. Through different characterization techniques (TEM, CO chemisorption), a strong Pt-Ceria interaction was evidenced, which helped in preventing Pt particle agglomeration under reaction conditions and promoted active interface sites. Both features are proposed to be responsible for the Pt/CeO2 catalysts better catalytic performance. The effect of the Pt precursor depends on the nature of the support. In ceria, Cl species benefited the generation of oxygen vacancies and surface ceria reducibility; both features are responsible for the Pt/CeO2 anti-coke properties, thus impacting positively in the catalytic performance of the Pt(-cl)/Ce sample. Conversely, in alumina, these Cl species triggered particle sintering and carbon deposition during the DRM reaction, affecting the Pt(-cl)/Al catalytic performance.
Resumen. Catalizadores de platino (1.5 % en peso) soportados sobre CeO2 y γ-Al2O3 fueron sintetizados mediante impregnación húmeda utilizando dos diferentes precursores de Pt: H2PtCl6 and Pt(acac)2. Los catalizadores fueron evaluados en la reacción de reformado seco de metano (DRM) en condiciones estequiométricas (razón molar de CH4/CO2 igual a 1) y con dos metodologías: en función de la temperatura de reacción (400-800 °C) y en función del tiempo de reacción (800 °C / 24 h). Los catalizadores de platino soportados sobre ceria mostraron las mejores propiedades catalíticas, especialmente en las pruebas de estabilidad, donde la desactivación fue muy baja. Por el contrario, la estabilidad catalítica de las muestras soportadas en alúmina fue considerablemente menor, debido tanto a la formación de residuos de carbón como al sinterizado de partículas de Pt. Por medio diferentes técnicas de caracterización (TEM, Quimisorción de CO), se evidenció una fuerte interacción Pt-Ceria, la cual ayudó a prevenir la aglomeración de partículas de Pt durante la reacción, además de promover la generación de sitios activos interfaciales. Ambas características se proponen como las responsables de las mejores propiedades catalíticas presentadas por los catalizadores Pt/CeO2. El efecto del precursor del Pt depende de la naturaleza del soporte. En ceria, las especies de cloro beneficiaron la generación de sitios vacantes de oxígeno así como la reducción superficial de la ceria; ambas características son responsables de las propiedades anti-coque en el sistema Pt/CeO2, por lo tanto, estas impactaron positivamente en el desempeño catalítico de la muestra Pt(-cl)/Ce. Por el contrario, en la alúmina, estas especies cloradas aparentemente promovieron el sinterizado de partículas y los depósitos de carbono durante la reacción, lo cual afectó el desempeño catalítico de la muestra Pt(-cl)/Al.
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