Tuning Ru/Ni sites in the perovskite-based precursor synthesis to make more efficient and durable dual-function materials for integrated CO2 capture and methanation

A new generation of Dual Function Materials (DFMs) were obtained after the controlled reduction of 20 % La0.6Ca0.4Ni0.95Ru0.05O3/CeO2 synthesized combining citric acid-wetness impregnation methods. Different parameters such as pH of the starting solution, calcination protocol were modified in order...

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Detalles Bibliográficos
Autores: Onrubia Calvo, Jon Ander, Pereda Ayo, Beñat, De La Torre Larrañaga, Unai, González Marcos, Jose Antonio, González Velasco, Juan Ramón
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/76617
Acceso en línea:http://hdl.handle.net/10810/76617
Access Level:acceso abierto
Palabra clave:CO2 methanation
ICCM technology
dual function material
perovskite precursor
Ru doping
Descripción
Sumario:A new generation of Dual Function Materials (DFMs) were obtained after the controlled reduction of 20 % La0.6Ca0.4Ni0.95Ru0.05O3/CeO2 synthesized combining citric acid-wetness impregnation methods. Different parameters such as pH of the starting solution, calcination protocol were modified in order to synthesize materials with variable nanostructure, surface chemistry and textural properties, thereby effectively tuning the material activity and stability for the integrated CO2 adsorption and in situ methanation operation. The samples were extensively characterized before and after catalytic tests by XRD, Raman, STEM-EDS, XPS, N2 adsorption-desorption, H2-TPR, H2-TPD, CO2-TPD, and H2-TPSR. It was found that the DFM obtained from the precursor prepared in absence of NH3 promoted Ru accommodation within the perovskite structure. The corresponding DFM showed enhanced textural properties, Ru/Ni actives sites accessibility and weak/medium basic sites concentration and, consequently, displayed the highest CH4 yield (312 µmol g−1) and fastest CH4 production kinetics under cycles of CO2 adsorption and in situ hydrogenation to CH4. Furthermore, this sample showed higher stability than conventional Ru-based DFMs, with CH4 production decreasing by less than 6 % compared to 25 % observed for conventional ones, due to a lower tendency for metal sintering, emerging as a promising alternative for long-term operation under realistic industrial conditions.