期刊
MACROMOLECULES
卷 51, 期 2, 页码 318-327出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.macromol.7b02608
关键词
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资金
- NHMRC-ARC Dementia Research Development Fellowship [APP1109945]
- Queensland University of Technology (QUT)
- Australian Research Council (ARC)
- Landesgraduierten Scholarship of the State of Baden-Wuerttemberg
- University of Warwick/Unilever studentship
- Australian Research Council (ARC) Centre of Excellence in Convergent Bio-Nano Science and Technology [CE140100036]
We report a high-resolution electrospray ionization mass spectrometric (HR ESI-MS) access route leading to in-depth insights into the spontaneous zwitterionic copolymerization mechanism between cyclic imino ethers (i.e., 2-methyl-2-oxazoline (MeOx), 2-ethyl-2-oxazoline (EtOx), or 2-ethyl-2-oxazine (EtOz)) with acrylic acid (AA), exploiting the characteristic species accumulating during the copolymerization as well as tandem mass spectrometry (MS/MS). We demonstrate preferences in alpha,omega-end group formation by screening various feed ratios of cyclic imino ethers and acrylic acid (e.g., MeOx:AA = 1:1; MeOx:AA = 2:1; and MeOx:AA = 1:2). Critically, a calibration curve-based on AA-MeOx-AA dimer-was established allowing for the semiquantitative determination of the end-group ratios with different feed ratios of acrylic acid. The formation of previously suggested alternating copolymers was confirmed by MS/MS experiments. Deviations from an ideal alternating composition were found to decrease from MeOx to EtOx to EtOz. The results of (semiquantitative) HR ESI-MS and MS/MS measurements suggest, for the first time presented in such precision, a polymerization mechanism for the spontaneous zwitterionic (alternating) copolymerization indicating optimal monomer ratios and pairings.
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