Turizo Pinilla, Edgar Eduardo

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    Exploring synergistic interactions in copper-gallium oxide-zirconium oxide catalysts for CO2 hydrogenation to methanol
    (2022-07-08) Turizo Pinilla, Edgar Eduardo; Pagán-Torres, Yomaira J.; College of Engineering; Cardona-Martínez, Nelson; Martínez-Iñesta, Maria M.; Department of Chemical Engineering; Tarafa Velez, Pedro
    The development of technologies for capturing, storing, and converting carbon dioxide to chemicals and fuels is critical for addressing issues arising from global climate change. The reduction of CO2 to chemicals such as methanol is attractive since it currently serves as a bulk platform chemical and an energy carrier. Industrially, methanol is produced from syngas mixtures (CO2/CO/H2) over Cu/ZnO/Al2O3 catalysts at elevated pressures and temperatures. However, Cu/ZnO/Al2O3 has shown limited productivity in the absence of CO and low stability because of catalyst sintering. In this work, the performance of copper/gallium oxide/zirconium oxide catalysts with varying Cu/Ga/Zr ratios was evaluated in the hydrogenation of CO2 to methanol at 240-300°C and 500 psi. This catalyst exhibited exceptional methanol productivities of >0.5 gMeOH/gcat/h under optimized reaction conditions and time-on-stream stability within a 24 h period. Catalyst characterization (hydrogen temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and scanning electron microscopy (SEM), N2O chemisorption), and kinetic studies were combined to determine the nature of the active sites and the reaction pathways by which copper- gallium oxide- zirconium oxide systems hydrogenate CO2 to methanol.