Abstract

ARBELAEZ PEREZ, Oscar Felipe et al. Gas phase synthesis of dimethyl carbonate from CO₂ and CH₃OH over Cu-Ni/AC. A kinetic study. Rev.fac.ing.univ. Antioquia [online]. 2020, n.95, pp.88-99. ISSN 0120-6230.  https://doi.org/10.17533/udea.redin.20190941.

The catalytic activity for dimethyl carbonate formation from carbon dioxide and methanol over mono and bimetallic Cu:Ni supported on activated carbon is presented. Bimetallic catalysts exhibit higher catalytic activity than the monometallic samples, being Cu:Ni-2:1 (molar ratio) the best catalyst; X-Ray diffraction, transmission electron microscopy, and metal dispersion analysis provided insight into the improved activity. In situ FT-IR experiments were conducted to investigate the mechanism of formation of dimethyl carbonate from methanol and carbon dioxide over Cu-Ni:2-1. The kinetics of the direct synthesis of dimethyl carbonate in gas phase over Cu:Ni-2:1 supported on activated carbon catalyst was experimentally investigated at 12 bar and temperatures between 90 °C and 130 °C, varying the partial pressures of CO2 and methanol. Experimental kinetic data were consistent with a Langmuir-Hinshelwood model that included carbon dioxide and methanol adsorption on catalyst actives sites (Cu, Ni and Cu-Ni), and the reaction of adsorbed CO2 with methoxi species as the rate determining step. The estimated apparent activation energy was 94.2 kJ mol-1.

Keywords : Methanol; catalysts; reaction mechanism; reaction rate; In situ FT-IR analysis.

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