Distribution of Alternating Sequences in Methyl Methacrylate/<i>n</i>-Butyl Acrylate Copolymers Prepared by Atom Transfer Radical Polymerization

Sosnowski, Stanisław; Szymański, Ryszard; Lorandi, Francesca; Olszewski, Mateusz; Sobieski, Julian; Yin, Rongguan; Matyjaszewski, Krzysztof

doi:10.1021/acs.macromol.1c01930

Cited by 22 publications

(32 citation statements)

References 47 publications

(70 reference statements)

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“…We recently reported the synthesis of SiO 2 - g -PBA- grad -PMMA particle brushes with various grafting densities using a semibatch copolymerization activator regenerated by electron transfer (ARGET) surface-initiated atom transfer radical polymerization (SI-ATRP) . The deliberate variation of monomer feed ratio and conversion ratio was shown to facilitate the synthesis of gradient and random copolymer brush particle architectures . A detailed analysis of the distribution of various comonomer sequences in the gradient and random copolymers was also recently reported .…”

Section: Resultsmentioning

confidence: 99%

“…The deliberate variation of monomer feed ratio and conversion ratio was shown to facilitate the synthesis of gradient and random copolymer brush particle architectures . A detailed analysis of the distribution of various comonomer sequences in the gradient and random copolymers was also recently reported . Here, two series of SiO 2 - g -PBA- grad -PMMA were prepared, i.e.…”

Section: Resultsmentioning

confidence: 99%

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Topologically Induced Heterogeneity in Gradient Copolymer Brush Particle Materials

Zhao

Wang

et al. 2022

Macromolecules

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A facile synthetic route toward silica brush particles with random and gradient copolymer grafts comprised of n-butyl acrylate (BA) and methyl methacrylate (MMA) using surface-initiated atom transfer radical polymerization (SI-ATRP) was developed. The effect of chain architecture on the structure and thermomechanical properties of copolymer-tethered brush particle films was investigated and compared to linear copolymer analogues. Random copolymer brush systems displayed a uniform and narrow glass transition, and the dependence of the glass-transition temperature followed a similar trend as for linear copolymers. In contrast, gradient brush materials featured a splitting of the glass-transition temperature with increasing MMA content along with a step-like increase of Young’s modulus and a decrease in ductility. The results were interpreted in terms of the effect of brush architecture on the microstructure of films. The results suggested a “molecularly uniform” microstructure in films of the random brush as well as linear random and linear gradient copolymer systems. In contrast, gradient brush systems featured a heterogeneous microstructure in which MMA-rich regions acted as “traps” that reduced chain mobility. The formation of compositional heterogeneity was rationalized by the “prescribed orientation” of gradient copolymer chains near the particle interface that amplified composition fluctuations and hence local segregation of repeat units. The results highlight the need for a better understanding of the role of “geometric constraints” on the physical properties of copolymer brush particle-based hybrid materials and the opportunity for multiple property enhancement by control of segment distribution in addition to the overall composition.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Topologically Induced Heterogeneity in Gradient Copolymer Brush Particle Materials

Zhao

Wang

et al. 2022

Macromolecules

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“…The use of dipolar interactions eliminates chemical and physical alterations and enables multiple recoveries without external intervention . Although ideally alternating MMA/nBA sequences are desired, semi-batch programmed monomer feeding will enhance the amount of alternating sequences …”

Section: Results and Discussionmentioning

confidence: 99%

Self-Healable Acrylic-Based Covalently Adaptable Networks

Wang

Liu

et al. 2022

Macromolecules

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Combining autonomous self-healing and reprocessing in one material offers an extended life span and enables shape configuration changes. We developed commodity poly((2-acetoacetoxy)ethyl methacrylate/methyl methacrylate/n-butyl acrylate) [p(AAEMA/MMA/nBA)] copolymer networks that are capable of both self-healing without intervention as well as reprocessing. The thermoplastic p(AAEMA/MMA/nBA) was obtained by copolymerizing (2-acetoacetoxy)ethyl methacrylate (AAEMA), methyl methacrylate (MMA), and n-butyl acrylate (nBA), followed by cross-linking with tristriaminoethyl amine (TREN) to form covalently adaptable networks (CANs). This copolymer network exhibits self-healability under ambient conditions and reprocessibility by compression molding at 120 °C. Using an array of thermo-mechanical and spectroscopic tools, these studies show that reprocessibility is achieved by the exchange reactions of dynamic cross-links, whereas self-healing is facilitated by the recovery of energetically favorable inter-chain van der Waals interactions accompanied by the reversible E ⇌ Z isomerization of the CC bonds in vinylogous urethane moieties of the network.

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“…Numerical simulations of PMMA/P n BA copolymers prepared by ATRP under various conditions revealed that the number of alternating sequences is maximized for a statistical copolymer with 1/1 MMA/ n BA composition. [ 92 ] Thus, a feeding strategy in which MMA is continuously fed into the polymerization mixture to obtain statistical copolymers should provide materials exhibiting more effective self‐healing ability.…”

Section: The 12 Principles Of Green Chemistry and Their Implementatio...mentioning

confidence: 99%

Toward Green Atom Transfer Radical Polymerization: Current Status and Future Challenges

et al. 2022

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Dedicated to Professor Klaus Muellen on the occasion of his 75th birthdayReversible-deactivation radical polymerizations (RDRPs) have revolutionized synthetic polymer chemistry. Nowadays, RDRPs facilitate design and preparation of materials with controlled architecture, composition, and functionality. Atom transfer radical polymerization (ATRP) has evolved beyond traditional polymer field, enabling synthesis of organic-inorganic hybrids, bioconjugates, advanced polymers for electronics, energy, and environmentally relevant polymeric materials for broad applications in various fields. This review focuses on the relation between ATRP technology and the 12 principles of green chemistry, which are paramount guidelines in sustainable research and implementation. The green features of ATRP are presented, discussing the environmental and/or health issues and the challenges that remain to be overcome. Key discoveries and recent developments in green ATRP are highlighted, while providing a perspective for future opportunities in this area.

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Distribution of Alternating Sequences in Methyl Methacrylate/n-Butyl Acrylate Copolymers Prepared by Atom Transfer Radical Polymerization

Cited by 22 publications

References 47 publications

Topologically Induced Heterogeneity in Gradient Copolymer Brush Particle Materials

Topologically Induced Heterogeneity in Gradient Copolymer Brush Particle Materials

Self-Healable Acrylic-Based Covalently Adaptable Networks

Toward Green Atom Transfer Radical Polymerization: Current Status and Future Challenges

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