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The radical chain-growth polymerization mechanism consists of three steps: initiation, propagation, and termination of polymerization. The polymerization initiates when a free radical generated from the radical initiator adds to the unsaturated bond in the monomer. The unpaired electron of the free radical and one π electron in the unsaturated bond creates a σ bond between the free radical and the monomer. As a result, the other π electron in the unsaturated bond converts this...
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The cationic polymerization mechanism consists of three steps: initiation, propagation, and termination. In the initiation step of the polymerization process, the π bond of a monomer gets protonated by the Lewis acid catalyst, which is formed from boron trifluoride and water. The protonation of the π bond generates a carbocation stabilized by the electron‐donating group. In the propagation step, the π bond of the second monomer acts as a nucleophile and attacks the...
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The conversion of alkenes to macromolecules called polymers is a reaction of high commercial importance. The structure of the polymer is defined by a repeating unit, while the terminal groups are considered insignificant. The average degree of polymerization represents the number of repeating units in the polymer molecule and is denoted by the subscript n.
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Chain-growth or addition polymerization is successive addition reactions of monomers with a polymer chain. In radical chain-growth polymerization, the reaction proceeds via a free-radical intermediate. The free radical is formed from radical initiators, which spontaneously generate free radicals by homolytic fission. Organic peroxides (such as dibenzoyl peroxide, as shown in Figure 1) or azo compounds are popular radical initiators. A low concentration ratio of radical initiator to monomer is...
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The skeletal structure of polymers synthesized via radical polymerization is always branched. For example, the polymerization of ethylene by radical polymerization results in a low-density grade of polyethylene with a heavily branched skeletal structure. Here, the radical site abstracts hydrogen from the growing chain, and the radical site shifts from the end (a primary carbon center) to anywhere within the growing chain (a secondary carbon center). Consequently, the part of the chain from the...
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3D Printing and In Situ Surface Modification via Type I Photoinitiated Reversible Addition-Fragmentation Chain Transfer Polymerization
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Free-Standing 3D Printing of Epoxy-Vinyl Ether Structures Using Radical-Induced Cationic Frontal Polymerization.

Brecklyn R Groce1, Alexandra V Aucoin1, Md Asmat Ullah2

  • 1Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803, United States.

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Summary

Frontal polymerization enables faster, more energy-efficient 3D printing of unsupported structures. This study developed a novel resin for radical-induced cationic frontal polymerization, demonstrating successful printing of complex free-standing geometries.

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Area of Science:

  • Polymer Chemistry
  • Additive Manufacturing
  • Materials Science

Background:

  • Frontal polymerization offers advantages in energy efficiency and printing speed for additive manufacturing.
  • It enables the creation of free-standing structures without the need for support materials.

Purpose of the Study:

  • To develop and optimize a resin system for radical-induced cationic frontal polymerization in 3D printing.
  • To investigate the effects of formulation components on front velocity and printability.
  • To demonstrate the capability of printing free-standing structures with complex geometries.

Main Methods:

  • A novel resin was formulated using epoxies, vinyl ether, and an initiating system (iodonium salt and peroxide).
  • Resin properties (reactivity, rheology, physical properties) were optimized for extrusion-based printing.
  • A modified desktop 3D printer controlled resin extrusion and deposition.
  • Free-standing printing of single filaments and helical geometries was achieved by coordinating UV initiation, air pressure, and printing speed.

Main Results:

  • The optimized resin frontally polymerized via radical-induced cationic mechanism, enabling free-standing structure printing.
  • Increased vinyl ether and cycloaliphatic epoxide content enhanced front velocity.
  • Carbon nanofibers boosted front velocity more than milled carbon fibers.
  • The resin with carbon nanofibers and fumed silica showed shear-thinning behavior, suitable for 4 wt% extrusion printing.
  • Transverse-printed specimens had lower flexural strength due to voids and adhesion issues.

Conclusions:

  • Frontal polymerization is a viable technique for energy-efficient, high-speed additive manufacturing of complex, unsupported structures.
  • Resin formulation, particularly the ratio of vinyl ether and cycloaliphatic epoxide, significantly influences front velocity.
  • Carbon nanomaterials, especially nanofibers, can enhance printing speed.
  • Careful control of printing parameters is crucial for achieving desired mechanical properties and successful free-form fabrication.