Abstract
The N,N,N‘,N‘,N‘ ‘-pentamethyldiethylenetriamine (PMDETA) ligand, commonly used in copper-catalyzed atom transfer radical polymerization (ATRP), is known to have an inhibitive effect on the kinetics of the ATRP of alkyl acrylate monomers due to the chain transfer reaction involving the ligand species. However, the exact chemical nature of the ligand radicals resulting from the chain transfer reaction and other reactions that the ligand radicals may undergo subsequently are presently unknown, making it difficult to establish the precise reaction mechanism of the copper/PMDETA-based ATRP of alkyl acrylate monomers. In an effort to gain a better understanding of the chemistries and reactions of the PMDETA species in the ATRP of n-butyl acrylate, we conducted (i) experimental measurements to determine how changes in PMDETA concentration influence the ATRP kinetics and the molecular properties of the product, (ii) electron density functional theory (DFT) calculations to identify probable pathways for reactions...
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