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DREAM REACTION FUNDED PROJECTS materials do not have any defined functional end groups, they are unsuitable for use in manufacturing polyurethanes. The research effort was focused on transition metal complexes of aluminium, iron, chromium and cobalt for which a library of selected ligands had been synthesised. The best result was achieved with a cobalt(III) catalyst that enabled the conversion of cyclohe- xene oxide to the corresponding polyether polycarbonate polyol with a yield of 43% and a molar carbonate-to-ether ratio of 49:1. In addition, alumini- um complexes with bis(phenoxide) ligands were developed that led to the 100% conversion of cyclohexene oxide, but produced less carbonate than ether product (carbonate-to-ether ratio was 1:5). Although these newly de- veloped complexes exhibited outstanding activity with respect to the con- version of cyclohexene oxide, none of them proved capable of converting propylene oxide to the copolymer. The most promising system identified for the copolymerisation of propylene oxide and CO2 was the double-metal cyanide (DMC) catalyst system (Figure 2), which has the general sum formu- la Zn3[Co(CN)6]2·ZnCl2·H2O·ROH, where R denotes an organic residue. The DMC catalyst system was developed further and resulted in an outstanding productivity of 5200–10700 g (PPP) per gram of catalyst at a selectivity of 94–98% and a catalyst load of the order of 100 ppm depending on require- ments, and was in some cases even greater. Fig. 8: Schematic representation of a double-metal cyanide catalyst (DMC). By carefully controlling the composition of the reaction system, the viscosi- ty and CO2-content could be varied across a wide range. By selecting diffe- rent starter molecules it also proved possible to synthesise copolymers with different functionalities, i.e. with different numbers of hydroxyl groups per polymer molecule. The aim of the subproject ‘Aromatic Carbonates’ was to develop an eco- nomical, phosgene-free synthetic route to diphenyl carbonate (DPC). The- se DPC molecules can then undergo further reaction with bisphenol A to produce polycarbonates. The subproject conducted research into catalytic systems that would be capable of catalysing the reaction between phenol and CO2 or CO to yield diphenyl carbonate. Experiments involving palla- dium-based catalyst candidates failed as it was not possible to stabilise the catalysts during the reaction. Direct carbonylation of phenol to DPC was achieved with the aid of novel heterobimetallic catalysts, but the activity displayed was low. Metal-free triazine-based catalysts were able to convert 35PDF Image | Chemical Processes and Use of CO2
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