Development of Efficient Ni-Based Catalysts for Co2 Methanation: Unraveling the Impact of Support Properties on Catalytic Performance

Abstract

It is widely recognized that the choice of support significantly influences the performance of Ni-based CO₂ methanation catalysts. This study systematically investigated how different supports affected catalytic properties, focusing on strong metal-support interactions, redox performance, and pore topology. To elucidate the impact of various supports on thermal decomposition behavior and reaction mechanisms, advanced techniques such as online-tandem TG-MS, in-situ DRIFTS, and online TPSR were employed to analyze the calcination of catalyst precursors and the CO₂ methanation process. The catalysts examined included Ni-based systems supported on metal oxides (e.g., MgO, γ-Al₂O₃, La₂O₃, CeO₂) and porous silica-based materials (e.g., SiO₂, ZSM-5, MCM-41, SBA-15, KCC-1, NS-MFI). Results demonstrated that the support choice profoundly affected the activity and stability of Ni-based catalysts. Notably, Ni/CeO₂ and Ni/NS-MFI exhibited exceptional low-temperature catalytic performance. The superior activity of Ni/CeO₂ was attributed to abundant oxygen vacancies, high Ni dispersion, and excellent redox properties of CeO₂, while Ni/NS-MFI's performance stemmed from the mesoporous confinement and microporous penetration effects of NS-MFI. Therefore, this study would provide valuable insights for the design and development of efficient Ni-based catalysts for CO₂ methanation.

Keywords: Support effects, Ni-based catalysts, Low-temperature CO2 methanation, In-situ and quasi-situ dynamic characterization techniques, Reaction intermediates and mechanism