Combined (CO2+CO) Hydrogenation with Methanolysis Using Aerosol Metal-Organic Framework-Derived Hybrid Catalysts

This study introduces a novel one-pot reaction system that efficiently converts greenhouse gases into methanol while simultaneously processing polyethylene terephthalate (PET) into dimethyl terephthalate (DMT) and ethylene glycol (EG). Our approach involves the development of hybrid materials derived from metal-organic frameworks (MOFs) using an aerosol-assisted synthesis method. These catalysts, which include a Cu/ZnO active phase on various supports, are optimized for the hydrogenation of both carbon monoxide (CO) and carbon dioxide (CO₂). By integrating PET methanolysis with the (CO₂ + CO) hydrogenation process, we achieved a significant enhancement in conversion ratios, exceeding 2.5 times their individual values. This synergistic approach effectively addresses the challenges posed by both plastic waste and greenhouse gas emissions. An impressive space–time yield of 5.6 mmol  g_cat⁻¹h⁻¹ and selectivity of 92 % for DMT production were achievable under optimized conditions. These results highlight the effectiveness of MOF-derived catalyst materials in facilitating complex chemical transformations and contribute significantly to environmental sustainability. This dual-function system offers a practical solution for the utilization of plastic waste and greenhouse gases, marking an important step toward a circular economy.