Effects of oxide carriers on surface functionality and process performance of the Cu–ZnO system in the synthesis of methanol via CO2 hydrogenation (original) (raw)

2013, Journal of Catalysis

AI-generated Abstract

Physicochemical properties and CO2-to-methanol hydrogenation functionality (T R , 453-513 K; P R , 0.1-5.0 MPa) of Al2O3-, ZrO2-, and CeO2-supported Cu-ZnO catalysts are systematically addressed. Carriers control texture and metal surface exposure (MSA), while characterization of steady-state catalysts shows extensive CO2 and H2 coverage regardless of MSA, proving a crucial influence of the oxide carrier on the adsorption properties of the Cu-ZnO system. The kinetic dependence on p CO2 and p H2 confirms that dioxo-methylene intermediate hydrogenation is the rate-determining step (r.d.s.) at P < 0.1 MPa, while a low kinetic dependence on pressure (0.3-0.5) signals that product desorption is the r.d.s. at P > 0.1 MPa. The influence of flow rate on selectivity pattern discloses that CH3OH is the primary reaction product at T < 473 K, while at higher temperatures, CO forms by consecutive decomposition of methanol (MD) and parallel reverse water-gas shift (RWGS). Textural and chemical effects of the zirconia carrier confer superior performance on the Cu-ZnO/ZrO2 system, attaining a space time yield (STY) of 1.2 kg CH3OH kg-1 cat h-1 at 10% conversion per pass.

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Effects of oxide carriers on surface functionality and process performance of the Cu–ZnO system in the synthesis of methanol via CO2 hydrogenation (original) (raw)

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