Access to smaller phase domain dimensions requires reducing the degree of polymerization, which weakens segregation and increases the importance of strong segmental incompatibility; however, the same chemical contrast can impede direct sequential block copolymerization through differences in solvent affinity. Here, we synthesized poly(hexafluorobutyl acrylate)-block-poly(acrylamide) (PHFBA-b-PAAm) in one pot from 2,2,3,4,4,4-hexafluorobutyl acrylate (HFBA) and acrylamide (AAm) using organotellurium-mediated radical polymerization (TERP), without intermediate purification or solvent exchange. Although AAm addition induced micron-scale aggregation at room temperature, the system reorganized into a nanoscale dispersion under polymerization conditions, supporting high-conversion chain extension with low dispersity. Well-defined block copolymers with molecular weights of 15–100 kDa and varied compositions were obtained at high monomer conversions. Small-angle X-ray scattering and atomic force microscopy revealed microphase separation throughout the series, including the 15 kDa sample. Overall, direct synthetic access and low-molecular-weight phase separation can be reconciled in block copolymers with strongly incompatible segments.
Developing sustainable polymer platforms requires simultaneous control over micro- and macromolecular structures, material properties, and end-of-life fate. Herein, we report the one-pot organocatalyzed group transfer copolymerization (O-GTcP) of dioctyl and diethyl muconates (DOM and DEM), achieving statistical copoly...
José David Estrada-Sotomayor, Thomas Dardé, Émilie Diomar et al.· Chemical Science· 0 citations
Thermoplastic elastomer gels constitute a valuable class of composition-tunable materials that are typically fabricated from styrenic ABA triblock copolymers (i) possessing a morphology with A-dispersions in a B-matrix and (ii) physically modified with a B-selective, low-volatility oil to controllably alter mechanica...
Kacie M. Wells, Alexey A. Gavrilov, Ivan Kuzmenko et al.· Macromolecules· 0 citations
Understanding the internal architecture of copolymer microgels is crucial for establishing how nanoscale polymer organization controls their stimuli-responsive behavior. Here we focus on thermoresponsive P(N-isopropylacrylamide-co-N-isopropyl-methacrylamide), P(NIPAM-co-NIPMAM), microgels with varying mole fraction of...
Jacopo Vialetto, F. Brasili, L. Tavagnacco et al.· 0 citations
Inducing phase separation in crosslinked polymer systems with high-molecular-weight block copolymers (BCP) has been shown to produce composites with enhanced tensile properties and unique thermomechanical behavior. However, detailed understanding of the relationships between BCP chemical composition and physical inte...
Tanner L. Grover, Jennafer M. Davis, Lars Nelson et al.· Macromolecules· 0 citations
The independent manipulation of chemical functionality over the equilibrium morphology in conventional block copolymer (BCP) self-assembly is intrinsically hindered due to the tight composition–structure coupling. Here, we report a synthesis strategy that breaks this constraint by employing self-assembled ABC tribloc...
Yuan-Zhi Li, Sarah A. Hesse, Wen-Lu Wang et al.· Journal of the American Chem...· 0 citations
Impedance mismatch block copolymers, combining rubbery polyisobutylene (PIB) with glassy polystyrene (PS) segments, show promise for the design of high-strain-rate material applications. However, the molecular-level processes of energy absorption and dissipation under high strain rates in the solution state are poorly...
Parth K. Vagholkar, Alexander J. Rosario, John F. Searles et al.· ACS Applied Polymer Material...· 0 citations
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