4.7 Article

Combined hydrogenation of CO2 and CO to methanol using Aerosol-Assisted Metal-Organic Framework-Derived hybrid catalysts

Journal

FUEL
Volume 349, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2023.128647

Keywords

Carbon dioxide; Carbon monoxide; Copper; Methanol; Aerosol

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In this study, a spray-drying approach was used to develop a Cu-based metal-organic framework (Cu-MOF) supported on aluminum oxide nanoparticle cluster, as well as its derived Cu-ZnO/Al2O3 hybrid catalyst for the combined hydrogenation of CO and CO2 to methanol. The catalyst showed high space time yield and selectivity to methanol under moderate pressure and relatively low temperature operation. Incorporation of ZnO and Al2O3 enhanced the dispersion and redox ability of Cu in the MOF-derived catalyst, both of which were critical factors to the catalytic activity. The study demonstrates a new route for the design of MOF-derived catalysts and shows promise for the catalysis of various chemical reactions in CO2 capture and utilization.
In this study, a spray-drying approach is presented to develop (1) Cu-based metal-organic framework (Cu-MOF) supported on aluminum oxide nanoparticle cluster and (2) its derived Cu-ZnO/Al2O3 hybrid catalyst for com-bined (CO + CO2) hydrogenation to methanol. The results show superior high space time yield, 23.14 mmol gcat- 1h-1, and selectivity to methanol (85%) were achievable under a moderate-pressure (30 bar) and relatively low -temperature (220 degrees C) operation. Incorporation of ZnO and Al2O3 (i.e., in the form of nanoparticle cluster) enhanced the dispersion and the redox ability of Cu in the MOF-derived catalyst, both of which were critical factors to the catalytic activity toward the combined hydrogenation of CO2 and CO to methanol. An optimal performance, in terms of the methanol yield, was achieved by using the catalyst with a Cu/Zn molar ratio of 2 and partially reduction by H2 at a relatively lower temperature (300 degrees C). The work demonstrates a new route for the design of MOF-derived catalyst by using an aerosol-assisted synthesis approach, showing promise for the catalysis of a variety of chemical reactions in the field of CO2 capture and utilization.

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