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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 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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Electrocyclic reactions, cycloadditions, and sigmatropic rearrangements are concerted pericyclic reactions that proceed via a cyclic transition state. These reactions are stereospecific and regioselective. The stereochemistry of the products depends on the symmetry characteristics of the interacting orbitals and the reaction conditions. Accordingly, pericyclic reactions are classified as either symmetry-allowed or symmetry-forbidden. Woodward and Hoffmann presented the selection criteria for...
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Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
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Radical substitution reactions can be used to remove functional groups from molecules. The hydrogenolysis of alkyl halides is one such reaction, where the weak Sn–H bond in tributyltin hydride reacts with alkyl halides to form alkanes. Here, the reagent Bu3SnH yields tributyltin halide as a byproduct.
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Reversing Blocking Order of Trithiocarbonate-Mediated RAFT Polymerizations Using Photocatalysis.

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Summary

Researchers developed a new method using photoinduced electron/energy transfer (PET) catalysis and trithiocarbonate (TTC)-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization to synthesize acrylic-methacrylic block copolymers, overcoming previous synthetic limitations.

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Block copolymersPhotocatalysisRAFTThermoplastic elastomerTrithiocarbonate

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Photocatalysis

Background:

  • Acrylic-methacrylic block copolymers are synthetically challenging to produce.
  • Existing methods have limitations in controlling block order and copolymer properties.

Purpose of the Study:

  • To develop a novel method for synthesizing acrylic-methacrylic block copolymers.
  • To overcome limitations in block order and improve copolymer uniformity.
  • To explore the impact of block order on material properties.

Main Methods:

  • Utilized photoinduced electron/energy transfer (PET) catalysis with trithiocarbonate (TTC)-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization.
  • Synthesized poly(methyl acrylate-b-methyl methacrylate) using a photocatalyst (fac-Ir(ppy)3).
  • Investigated the effect of tertiary amines on radical stabilization and copolymer uniformity.

Main Results:

  • Achieved predictable molecular weight increases with conversion using PET-RAFT.
  • Demonstrated improved block copolymer uniformity (Đ < 1.47) with the addition of a tertiary amine.
  • Synthesized high molecular weight triblock copolymers with exceptional strain (>1600%) properties.

Conclusions:

  • A new methodology for synthesizing acrylic-methacrylic block copolymers using TTCs and photocatalysis has been established.
  • Insights into photocatalyst-mediated radical polymerization kinetics and radical stabilization were gained.
  • New high-performance polymeric materials with tunable properties based on block order were synthesized.