Mechanochemical Synthesis of High-Entropy MOF-74 with Multiple Active Sites for CO₂ Adsorption and Synergistic Conversion

Abstract

Compared with monometallic metal–organic frameworks (MOFs), the synergistic effect of multiple metals significantly enhances the catalytic performance of the CO 2 cycloesterification reaction, leading to improved CO 2 adsorption and catalytic conversion capabilities. To investigate this concept, a high-entropy MOF-74 (HE-MOF-74) with a uniform distribution of five distinct metal ions (Zn 2+, Mg 2+, Ni 2+, Co 2+, and Cu 2+ ) was successfully synthesized using a straightforward mechanical ball milling technique and comprehensively characterized (including structural, morphological, and physicochemical properties). The results reveal that HE-MOF-74 exhibits significantly increased specific surface area and CO 2 adsorption capacity compared with those of monometallic MOF-74. The presence of multiple unsaturated metal centers as Lewis acid sites, oxygen atoms linking the metals, and ligand-based hydroxyl groups serving as base sites enable efficient immobilization of CO 2 into cyclic carbonate. This study introduces a novel synthetic approach for the green and efficient production of HE-MOF-74 and proposes a new application for CO 2 utilization.