Abstract

A one pot catalytic system which involves Cu and an alkoxide co-catalyst has been used for methanol (MeOH) synthesis at low temperature. Up to about 92% syngas conversion per pass and more than 90% selectivity to MeOH (the rest is methyl formate) was obtained depending on the amount of catalyst employed at 100°C and 20bar syngas pressure. Low temperature methanol synthesis presents a good alternative to current technology for methanol production since the former is thermodynamically favored and gives a high yield per pass. Cu particles sized around 10±5nm were found to be involved in the catalytic process. Cu nanoparticles of increasing size was synthesized by varying temperature. However, methanol production decreased with increasing Cu nanoparticle size. Moreover, the maximum conversion at the end of each successive batch declined as a function of the number of cycles performed. Decrease in catalyst activity corresponded to Cu nanoparticle densification, suggesting agglomeration to be a major catalyst deactivation pathway.

Highlights

  • Methanol (MeOH) has been identified as a potential multipurpose molecule for energy and CO2 storage [1]

  • Up to about 92% syngas conversion per pass and more than 90% selectivity to MeOH was obtained depending on the amount of catalyst employed at 100 °C and 20 bar syngas pressure

  • A low temperature methanol synthesis (LTMS) reaction was identified by Christiansen in 1919 [6], which presented the possibility of almost full syngas conversion to MeOH per pass at low temperature

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Summary

Introduction

Methanol (MeOH) has been identified as a potential multipurpose molecule for energy and CO2 storage [1]. MeOH is currently synthesized from syngas (made up of CO/CO2/ H2) over Cu/ZnO/Al2O3 catalysts, which operate at 250 °C and 70–100 bar of pressure [3,4] Though this technology is highly optimized, it is capital intensive and syngas conversion per pass is thermodynamically limited. A low temperature methanol synthesis (LTMS) reaction was identified by Christiansen in 1919 [6], which presented the possibility of almost full syngas conversion to MeOH per pass at low temperature (120 °C) conditions. This approach is known to involve firstly, carbonylation of methanol to form methyl formate (MF) and secondly, MF hydrogenolysis to form MeOH as indicated in Eqs.

Materials and experimental setup
Copper catalyst preparation
Catalytic testing
Cu catalyst characterization
Results and discussion
Deactivation test of the catalyst system
Varying Cu catalyst particle sizes with temperature
Conclusion
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