Catalytic Conversion of CO₂ to Methane Using Nickel‐Functionalized Mesoporous SBA‐1 with 3D Cage‐Type Porous Structure

Abstract Developing efficient heterogeneous catalysts for activating CO 2 is of considerable interest for achieving carbon neutrality. Therefore, many researchers have devoted a lot of effort to design and develop various porous materials‐based catalysts for CO 2 conversion. Catalysts with high activity and stability for CO 2 conversion are crucial for easy commercialization, but it remains a significant challenge to develop these catalysts. Herein, we report the fabrication of Ni‐functionalized mesoporous silica with 3D mesoporous structure, cage‐type pores, and different Ni contents for achieving enhanced CO 2 methanation and stability. The highly ordered mesoporous structure of SBA‐1 offers a high surface area (1315 m 2 g −1 ) that helps to anchor a significant amount of nickel nanoparticles. Insight into the structure of the catalyst and fine‐tuning of metal‐support interaction were in‐depth, characterized by the combination of X‐ray diffraction, electron imaging, and spectroscopic tools. The prepared Ni‐functionalized SBA‐1 materials exhibit an ordered mesoporous structure and the specific surface area decreases with increasing the concentration of the Ni on the porous channels of SBA‐1. The optimized Ni‐functionalized SBA‐1 yielded 80.1% conversion with a CH 4 selectivity of 96.9% at a gas hourly space velocity (GHSV) of 21,000 mLg cat −1 h −1 under the optimized reaction conditions. Temperature‐programmed surface reaction (TPSR) studies suggest a mechanism involving CO 2 dissociation into CO. The Ni‐loaded SBA‐1 catalyst demonstrated remarkable stability over five consecutive 24 h cycles, indicating its promising potential for practical application in sustainable energy production and greenhouse gas mitigation.