Replacing Cu(II)Br2 with Me6-TREN in Biphasic Cu(0)/TREN Catalyzed SET-LRP Reveals the Mixed-Ligand Effect

Xiaojing Feng, Devendra S. Maurya, Nabil Bensabeh, Adrian Moreno, Takahiro Oh, Yuqing Luo, Jā Nis Lejnieks, Marina Galià, Yoshiko Miura, Michael J. Monteiro, Gerard Lligadas, Virgil Percec

研究成果: Contribution to journalArticle

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The mixed-ligand system consisting of tris(2-aminoethyl)amine (TREN) and tris(2-dimethylaminoethyl)amine (Me6-TREN) during the Cu(0) wire-catalyzed single electron transfer-living radical polymerization (SET-LRP) of methyl acrylate (MA) in "programmed" biphasic mixtures of the dipolar aprotic solvents NMP, DMF, and DMAc with H2O is reported. Kinetic and chain end analysis studies by NMR and MALDI-TOF before and after thio-bromo "click" reaction demonstrated that Me6-TREN complements and makes the less expensive TREN a very efficient ligand in the absence of externally added Cu(II)Br2. Statistical analysis of the kinetic data together with control experiments demonstrated that this mixed-ligand effect enhanced the apparent rate constant of propagation, monomer conversion, and molecular weight control. The most efficient effect was observed at a 1/1 molar ratio between these two ligands, suggesting that in addition to a fast exchange between the two ligands, a new single dynamic ligand generated by hydrogen bonding may be responsible for the mixed ligand observed.

元の言語英語
ページ(範囲)250-261
ページ数12
ジャーナルBiomacromolecules
21
発行部数1
DOI
出版物ステータス出版済み - 1 13 2020

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Biomaterials
  • Polymers and Plastics
  • Materials Chemistry

フィンガープリント Replacing Cu(II)Br<sub>2</sub> with Me<sub>6</sub>-TREN in Biphasic Cu(0)/TREN Catalyzed SET-LRP Reveals the Mixed-Ligand Effect' の研究トピックを掘り下げます。これらはともに一意のフィンガープリントを構成します。

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    Feng, X., Maurya, D. S., Bensabeh, N., Moreno, A., Oh, T., Luo, Y., Lejnieks, J. N., Galià, M., Miura, Y., Monteiro, M. J., Lligadas, G., & Percec, V. (2020). Replacing Cu(II)Br2 with Me6-TREN in Biphasic Cu(0)/TREN Catalyzed SET-LRP Reveals the Mixed-Ligand Effect. Biomacromolecules, 21(1), 250-261. https://doi.org/10.1021/acs.biomac.9b01282