The Synergistic Effect of Pore Architect and Reducibility in Ceria-Promoted Ni Molecular Sieve for Methane Dry Reforming

Abstract

Methane and carbon dioxide, the primary contributors to global warming, are now at critical levels, threatening the extinction of numerous organisms on our planet. In this regard, dry reforming of methane reactions have gained considerable attention because of the conversion capacity of CH4 and CO2 into synthetic/energy-important syngas (H2 and CO). Herein, a molecular sieve (CBV3024E; SiO2/Al2O3 = 30) with ZSM-8-type pore architect, is utilized as the support for the active site of Ni and Ce promoters. Catalysts are characterized by surface area and porosity, X-ray diffraction study, Raman and infrared spectroscopy, thermogravimetry analysis, and temperature-programmed reduction/desorption techniques. A total of 2 wt.% ceria is added over 5Ni/CBV3024E to induce the optimum connectivity of aluminum in the silicate framework. NiO residing in these porous cages are mostly under “prominent interaction with support” which is reduced easily into metallic Ni as the active sites for DRM reactions. The active sites over 5Ni2Ce/CBV3024E remain stable during the DRM reaction and achieve ~58% H2 yield after 300 min TOS at 42,000 mL/(gcat.h) GHSV and ~70% H2 yield after 20 h at 26,000 mL/(gcat.h) GHSV. The high activity after a longer time stream justifies using CBV3024E molecular sieves as the support and ceria as the promoter for Ni-based catalyst towards the DRM reaction.