Comparative study on La-promoted Ni/γ-Al2O3 for methane dry reforming – spray drying for enhanced nickel dispersion and strong metal–support interactions

Abstract

Dry reforming of methane (DRM) enables an efficient utilization of two abundant greenhouse gases by converting them into syngas, a versatile feedstock for chemical synthesis. Aiming for high catalyst performance and enhanced coke resistance, different preparation techniques of La-promoted Ni/γ-Al₂O₃ catalysts for DRM were compared facilitating structure–performance correlations. The studied synthesis techniques comprehend incipient wetness impregnation and co-precipitation as well as alternative techniques such as spray drying. All catalysts were fully characterized before and after reaction by N₂-physisorption, XRD, H₂-TPR and STEM-EDX elemental mapping. Additionally, a thorough investigation of carbon deposits has been carried out by TGA/DSC and STEM-EDX, respectively. The different preparation techniques led generally to very different physical properties, structure, chemical species and anti-coking properties of the catalyst. However, some catalysts with similar physicochemical characteristics differed in catalytic performance and coking resistance. Superior catalytic performance could be reached for catalysts prepared by spray drying and related to excellent Ni dispersion, strong metal–support interaction and very low coke formation of only 2.7% of the catalyst weight. After 6 h time on stream only minor sintering occurred, with few Ni nanoparticles up to 10 nm.