Structure-Activity Relationship of Metal-Organic Frameworks-Derived Ni–Al Catalysts for CO Methanation Under Pyrolysis Strategy

Abstract

The conversion of metal-organic frameworks (MOFs) to MOF-derived composites via pyrolysis strategies can effectively address the shortcomings of MOFs, such as the small number of catalytic active sites and poor chemical stability, which limit practical catalytic applications. This article presents a series of Ni/MOF-derived composite materials with distinct morphologies, obtained by varying the calcination temperature. The NiO/M-Al 900 catalysts, calcined at 900 °C, form a NiO structure supported by NiAl₂O₄, which enhances the Ni–Al interaction. This catalyst inherits the high specific surface area (143.23 m² g⁻¹) and rich pore structure of the MOF, resulting in superior catalytic performance with CO conversion and CH₄ selectivity reaching 100% and 67%, respectively, and maintaining high activity under a 90 h stability test. The optimal Ni–Al interaction and the synergistic effect of the porous structure improve the dispersion and utilization of the active components, preventing sintering and carbon deposition of the catalysts during the reaction. This discovery provides a novel approach to designing high-performance multiphase MOF-derived composites for practical catalytic processes.