Abstract
A series of amine-bridged bis(phenolate) rare-earth (Sc, Y) aryloxides were synthesized and characterized. These complexes were successfully used for the controlled Lewis pair polymerization (LPP) of functional acrylamides in combination with phosphines, affording a new type of polyacrylamides with predictable molecular weight and low molecular weight distribution. The living nature of this LPP was verified by near-quantitative initiation efficiencies, a linear increase of molecular weight vs monomer-to-initiator ratio and monomer conversion, chain extensions, and the synthesis of well-defined block copolymers. The mechanistic studies were performed through the isolation of a zwitterionic intermediate as well as the end-chain analysis of oligomers, showcasing a rare-earth/phosphine cooperation. Furthermore, the resultant polyacrylamides exhibit outstanding thermal stability and great potential for application in photovoltaic devices.
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