Conference Paper

Direct synthesis of dimethyl carbonate from methanol and carbon dioxide: A thermodynamic and experimental study

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Abstract

The direct synthesis of dimethyl carbonate from carbon dioxide and methanol is an atom economic, green and promising process. The present work focuses on the same using calcined hydrotalcite supported on hexagonal mesoporous silica as a catalyst and phosphonium based ionic liquid as promoter. Ionic liquids are good solvents for many substances and have shown good results as promoters for the catalyst. The phosphonium based ionic liquids are good alkali promoters. Different modified Keggin type heteropoly acids supported on hexagonal mesoporous silica were also compared, which gives a good comparison between acid and base catalysts. The conversion, selectivity and yields were measured as a function of the amount of reactants, reaction time, temperature, pressure and amount of a catalyst. The experimental results were compared with the thermodynamic studies. Finally the kinetic model was developed by proposing a plausible reaction mechanism. Sustainability of the process was justified by using a supported hydrotalcite catalyst and by avoiding the use of harmful organic solvents in the presence of an ionic liquid with supercritical CO2. Key words: Carbon dioxide, Dimethyl carbonate, Ionic liquids, Supercritical CO2, Calcined Hydrotalcite, Heteropoly acids.

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Article
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This paper suggested multicriteria based evaluation tool to assess the sustainability of three different reaction routes to dimethyl carbonate: direct synthesis from carbon dioxide and methanol, transesterification of methanol and propylene carbonate, and oxidative carbonylation of methanol. The first two routes are CO 2-based and in a research and development phase, whereas the last one is a commercial process. The set of environmental, social, and economic indicators selected were renewability of feedstock, energy intensity, waste generation, CO 2 balance, yield, feedstock price, process costs, health and safety issues of feedstock, process conditions, and innovation potential. The performance in these indicators was evaluated with the normalized scores from 0 to +1; 0 for detrimental and 1 for favorable impacts. The assessment showed that the transesterification route had the best potential toward sustainability, although there is still much development needed to improve yield. Further, the assessment gave clear understanding of the main benefits of each reaction route, as well as the major challenges to sustainability, which can further aid in orienting development efforts to key issues that need improvement. Finally, it was concluded that a multicriteria analysis such as the one presented in this paper was a viable method to be used in the process design stage.
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