A new approach to network heterogeneity: Polymerization induced phase separation in photo-initiated, free-radical methacrylic systems

Caroline R. Szczepanski, Carmem Pfeifer, Jeffrey W. Stansbury

Research output: Contribution to journalArticle

33 Citations (Scopus)

Abstract

Non-reactive, thermoplastic prepolymers (poly- methyl, ethyl and butyl methacrylate) were added to a model homopolymer matrix composed of triethylene glycol dimethacrylate (TEGDMA) to form heterogeneous networks via polymerization induced phase separation (PIPS). PIPS creates networks with distinct phase structure that can partially compensate for volumetric shrinkage during polymerization through localized internal volume expansion. This investigation utilizes purely photo-initiated, free-radical systems, broadening the scope of applications for PIPS since these processing conditions have not been studied previously. The introduction of prepolymer into TEGDMA monomer resulted in stable, homogeneous monomer formulations, most of which underwent PIPS upon photo-irradiation, creating heterogeneous networks. During polymerization the presence of prepolymer enhanced autoacceleration, allowing for a more extensive ambient cure of the material. Phase separation, as characterized by dynamic changes in sample turbidity, was monitored simultaneously with monomer conversion and either preceded or was coincident with network gelation. Dynamic mechanical analysis shows a broadening of the tan delta peak and secondary peak formation, characteristic of phase-separated materials, indicating one phase rich in prepolymer and another depleted form upon phase separation. In certain cases, PIPS leads to an enhanced physical reduction of volumetric shrinkage, which is attractive for many applications including dental composite materials.

Original languageEnglish (US)
Pages (from-to)4694-4701
Number of pages8
JournalPolymer (United Kingdom)
Volume53
Issue number21
DOIs
StatePublished - Sep 28 2012

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Free radicals
Phase separation
Free Radicals
Polymerization
Monomers
Heterogeneous networks
Glycols
Dental composites
Dental materials
Turbidity
Dynamic mechanical analysis
Gelation
Phase structure
Homopolymerization
Thermoplastics
Irradiation
Composite materials
Processing

Keywords

  • Dental materials
  • Phase separation
  • Photopolymerizations

ASJC Scopus subject areas

  • Organic Chemistry
  • Polymers and Plastics

Cite this

A new approach to network heterogeneity : Polymerization induced phase separation in photo-initiated, free-radical methacrylic systems. / Szczepanski, Caroline R.; Pfeifer, Carmem; Stansbury, Jeffrey W.

In: Polymer (United Kingdom), Vol. 53, No. 21, 28.09.2012, p. 4694-4701.

Research output: Contribution to journalArticle

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