Advanced metal–support interactions in Cu/ZnO catalysts: the role of MOFs and ZrO2 for enhanced methanol production

Abstract

This study explores the role of metal–support interactions (MSI) and the incorporation of Metal–Organic Frameworks (MOFs) in enhancing the catalytic performance of Cu/ZnO-based catalysts, promoted and supported by Al₂O₃ (ANC) and ZrO₂ (ZNC), for CO₂ hydrogenation to methanol. The ZNC catalyst exhibits significantly superior catalytic performance, achieving up to 90% methanol selectivity and 28% CO₂ conversion under optimal conditions. These improvements are attributed to its higher dispersion, better reducibility, and stronger metal–support interaction (MSI), facilitated by the incorporation of ZrO₂. The use of MOFs in the catalyst synthesis contributes to enhanced stability and active site dispersion. The MSI, coupled with the presence of ZrO₂, facilitates hydrogen spillover, oxygen vacancy formation, and improved CO₂ and H₂ activation. DFT calculations corroborate experimental findings, revealing ZNC's lower activation energy barriers and more efficient pathways for methoxy intermediate formation. This study highlights the critical role of MSI and MOFs in optimizing catalytic efficiency, establishing ZNC as a promising candidate for sustainable methanol production.