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1CO2 UTILIZATION CO2ASAPOLYMERBUILDINGBLOCK of carbon dioxide and cyclohexene oxide.4,5 With a turnover frequency of 155,000 h-1 and molar masses of up to 350 kg/mol, complex 2 is the most active catalyst discovered thus far for the production of poly(cyclohexene carbonate).5 Fig. 11: Active catalysts for the copolymerization of CO2 and cyclohexene oxide Fig. 12: Stable six-membered resting state during CO2/PO copolymerisation Kinetic studies on complex 1 showed a first-order dependence on catalyst concentration. This indicates that both metal centres are involved in the rapid formation of the copolymer. Further studies of the effect of carbon dioxide pressure and epoxide concentration indicate that the mechanistic behaviour is clearly very different to that known from studies of mononu- clear complexes. A strong dependence on the CO2 concentration in solution was also observed. The concentration of epoxide was not found to be signifi- cantly rate limiting. Increasing the pressure of carbon dioxide can, however, reverse this finding. This is believed to be due to the rapid ring opening of the epoxide by the catalyst, making CO2 diffusion or insertion more rate li- miting.4 However, under the conditions tested, neither of the catalysts 1 or 2 showed any activity for the copolymerisation of CO2 and propylene oxide. Terpolymerisation experiments involving PO/CHO/CO2 and theoretical computations by P. Degelmann showed that after the initial single opening of the epoxide ring an alkoxide carbonato species forms, which in the case of the PO/CO2 copolymerisation represents the resting state of the catalytic cycle. The activation barrier for the subsequent CO2 insertion (104.8 kJ/mol) is significantly higher than that in the CHO/CO2 copolymerisation reaction (65.9 kJ/mol).6 40PDF Image | Chemical Processes and Use of CO2
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