Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 7, Issue 13, Pages 2897-2905Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7cy00383h
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Funding
- BMBF in the Project CO2 als Polymerbaustein [FKZ 01 RC 0902A]
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The copolymerization of carbon dioxide (CO2) with propylene oxide (PO) mediated by a nanoscopic zinc glutarate (ZnGA) catalyst was systematically analyzed using a design of experiments approach. The influence of the reaction temperature, CO2-pressure and reaction time on the catalyst's activity, the polymer composition and the molecular weight was determined. The empirical models obtained allow accurate predictions of the output parameter within the design space. The best catalyst performance in terms of polymer yield and CO2 incorporation was observed at molar fractions of x(CO2) approximate to 0.3 in the feed. The highest productivities were observed at 70-80 degrees C and pressures between 3.5 and 4.0 MPa. The copolymerization in bulk initially shows a pseudo-living behavior until M-n reaches a threshold of about 80 kDa. The polymerization rate at higher conversions seems to be limited too, possibly by the initiation of new chains; catalyst deactivation over time was excluded. The high PDI values at early reaction stages indicate that the initiation reaction is the rate-determining step.
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