Journal
FUEL
Volume 285, Issue -, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2020.119083
Keywords
CO2; Dimethyl carbonate; Manganese/cerium catalyst; Structure-activity relation; Chemical equilibrium modeling
Categories
Funding
- Ministry of Education, Science and Sport of Republic of Slovenia through EU European Fund for Regional Development [C3330-19-952015]
- Slovenian Research Agency through the Programme Chemistry for Sustainable Development [P1-0134]
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This study prepared various manganese-cerium catalysts using a surfactant-template method and tested their catalytic activity in DMC synthesis under CO2 pressure. The results showed that the catalytic activity is closely related to the acidic and basic sites of the catalysts, with Ce-1-Mn-0.125 catalyst exhibiting the highest basicity and acidity.
The relationships between structure and activity in heterogeneous catalysis have created a demand for new preparation routes for improved surface properties. In the present study, a number of Manganese-Cerium catalysts with varying manganese contents were prepared using a surfactant-template method and tested for CO2 conversion in dimethyl carbonate (DMC) synthesis at elevated temperature and CO2 pressure. The ManganeseCerium catalysts were characterized by N-2-sorption, XRD, CO2-TPD, NH3-TPD, SEM, TEM and Raman spectroscopy. The catalytic activity was closely related to the acidic and basic sites of the synthesized catalysts. The basic sites are responsible for the activation of CO2 and contribute to the formation of methoxy groups in the reaction. The weak and moderate acidic sites are responsible for the activation of methanol. It was found that the Ce-1-Mn-0.125 catalyst has the highest basicity and acidity compared to Ce-1-Mn-0.25 and Ce-1-Mn-1 catalysts. The optimization of the reaction conditions was investigated batchwise at various reaction parameters including reaction time and temperature. The reusability of the catalyst and the effect of the amount of manganese on the catalytic activity of Manganese-Cerium catalysts were also investigated. In addition, the calculation of the Gibbs free energy and heat of reaction was performed using chemical equilibrium modeling.
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