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Syntheses of Heterometallic Neodymium-Zinc Complexes and Their Performance in the Copolymerization of CO2 and Cyclohexene Oxide.

A series of Nd-Zn heterometallic complexes bearing o-phenylenediamine-bridged tris(phenolato) ligands (L) were synthesized and characterized. By tuning the backbones of ancillary tris(phenolato) ligands and initiating benzyloxy groups, a Nd-Zn heterometallic complex 12 (ClLNdZnOBnCF3) was found to be highly active for the copolymerization of CO2 and cyclohexene oxide (CHO) to produce perfect alternating poly(cyclohexene carbonate) with a high turnover frequency up to 5640 h-1 under the polymerization of 90 °C and 20 bar CO2 pressure. The kinetics study showed that CO2/CHO copolymerization catalyzed by 12 was the first order dependence of 12 and CHO concentration and the zero-order dependence of CO2 pressure. The reaction of 12 with CO2 generated a carbonate-coordinated [NdZnNd] trinuclear complex 13, which was believed to be the key intermediate to initiate CO2/CHO copolymerization. On the basis of some experiments, a plausible synergistic polymerization mechanism was proposed.