Effect of stereochemistry on nanoscale assembly of ABA triblock copolymers with crystallizable blocks

Yin, Xuechen; Hewitt, David; Zheng, Bingqian; Quah, Suan P.; Stanley, Christopher B.; Grubbs, Robert B.; Bhatia, Surita R.

doi:10.1016/j.polymer.2021.123683

Cited by 5 publications

(4 citation statements)

References 53 publications

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“…Ellipsoidal model better corresponds to the experimental data ( χ 2 values of 1.080, 1.078, and 0.902 instead of 1.217, 1.235, and 0.977), indicating a globule structure for ε‐PL and ε‐PL‐PLA as more probable compared to a coil. Due to similar values of scattering length density of PL and PLA (see Section 2), we used the model of the uniform ellipsoid instead of core‐shell ellipsoid model used in References 19.…”

Section: Resultsmentioning

confidence: 99%

“…For copolymers PL:PLA = 90:10 (w/w) copolymer PL:PLA = 50:50 (w/w), partial specific volume could be estimated as 0.1

v ̄

PLA + 0.9

v ̄

PL = 1.0688 Å 3 /Da and 0.5

v ̄

PLA + 0.5

v ̄

PL = 1.0425 Å 3 /Da, correspondingly. Due to the similar electron densities (and hence scattering length densities) of ε‐PL and L‐PLA, we used a homogeneous ellipsoid model instead of the core–shell ellipsoid model used in References 19 to fit SAXS data from copolymer micelles.…”

Section: Methodsmentioning

confidence: 99%

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Chemical transformations during mechanoactivation of ε‐polylysine‐poly‐L‐lactic acid mixture to obtain amphiphilic copolymers

Khaptakhanova,

Uspenskii,

Aleksandrov

et al. 2024

J of Applied Polymer Sci

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In this study presents a new strategy for the preparation of amphiphilic copolymers of ε‐polylysine (PL) and poly‐L‐lactic acid (PLA) using one‐step pulsed mechanochemical approach. Correlation between the synthesis parameters (ratio of homopolymers) and the structure of the resulting copolymers has been studied. The interaction products were characterized by nuclear magnetic resonance, Infrared spectroscopy, size‐exclusion chromatography, by varying the mass ratio of the initial homopolymers (PL:PLA = 10:90; 50:50; 90:10). It is shown that the largest number of product yield is formed in a ratio of homopolymers of 50:50, according to the reaction of aminolysis of polyesters. The dynamic light scattering method, transmission electron microscopy, and small‐angle x‐ray scattering were used to characterize nanoscale structures of copolymer macromolecules in aqueous solvent. As a result of pulsed mechanochemical action at all three ratios of homopolymers (PL:PLA = 10:90; 50:50; 90:10 w/w), the aminolysis reaction of the ester group occurs and branched macromolecules of copolymers are formed, which consist of chemically related sequences of homopolymers—main chain—PL, side branches—PLA. However, the maximum yield of the amphiphilic copolymer was 90 wt% with a PL:PLA ratio of 50:50. This study can serve as the development of important areas: deepen knowledge in the field of mechanochemical synthesis of amphiphilic copolymers.

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Section: Resultsmentioning

confidence: 99%

“…For copolymers PL:PLA = 90:10 (w/w) copolymer PL:PLA = 50:50 (w/w), partial specific volume could be estimated as 0.1

v ̄

PLA + 0.9

v ̄

PL = 1.0688 Å 3 /Da and 0.5

v ̄

PLA + 0.5

v ̄

Section: Methodsmentioning

confidence: 99%

Chemical transformations during mechanoactivation of ε‐polylysine‐poly‐L‐lactic acid mixture to obtain amphiphilic copolymers

Khaptakhanova,

Uspenskii,

Aleksandrov

et al. 2024

J of Applied Polymer Sci

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“…Interestingly, for our samples, this increase is more pronounced for the samples with smaller PEtG blocks, suggesting that other factors may be influencing the excess scattering at low q . Our VSANS results (Figure S11) suggest formation of large-scale structure in some samples, which has also been observed for associative hydrogels of ABA block copolymers with poly(lactic acid) (PLA) end-blocks, PLA–PEO–PLA . If such large structures are present, this would complicate interpretation of the low q scattering, as it would not solely be due to intermicellar attraction.…”

Section: Resultsmentioning

confidence: 99%

“…Our VSANS results (Figure S11) suggest formation of large-scale structure in some samples, which has also been observed for associative hydrogels of ABA block copolymers with poly(lactic acid) (PLA) end-blocks, PLA− PEO−PLA. 34 If such large structures are present, this would complicate interpretation of the low q scattering, as it would not solely be due to intermicellar attraction.…”

Section: Sans Analysismentioning

confidence: 99%

Aqueous Assembly and Hydrogel Rheology of Sustainable Glyoxylate-Based Copolymers

Yin

Hewitt

Zheng

et al. 2022

ACS Appl. Polym. Mater.

Self Cite

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The self-assembly of poly(ethyl glyoxylate)−poly(ethylene oxide)−poly(ethyl glyoxylate) (PEtG−PEO−PEtG) triblock copolymers in aqueous environments was systematically studied by using rheology and small-angle neutron scattering (SANS). These systems form associative micellar gels in water, with the PEtG end-blocks forming micelle cores and the PEO midblocks forming loops in the micelle coronas and intermicellar bridges. As PEtG block length is increased, rheology shows slower relaxation behavior, consistent with a longer lifetime of intermicellar bridges and associations. The length of the self-immolative PEtG block can be used to tailor the mechanical properties, size of nanoscale hydrophobic domains, and larger-scale assembly behavior of the block copolymer gels. These results can guide the design of self-immolative block copolymers with desirable rheological properties and nanoscale structures for a variety of applications.

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Influence of chain topology on gel formation and direct ink printing of model linear and star block copolymers with poly(ethylene oxide) and poly(ε-caprolactone) semi-crystalline blocks

Centeno,

Peñas,

Zhang

et al. 2023

European Polymer Journal

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Effect of stereochemistry on nanoscale assembly of ABA triblock copolymers with crystallizable blocks

Cited by 5 publications

References 53 publications

Chemical transformations during mechanoactivation of ε‐polylysine‐poly‐L‐lactic acid mixture to obtain amphiphilic copolymers

Chemical transformations during mechanoactivation of ε‐polylysine‐poly‐L‐lactic acid mixture to obtain amphiphilic copolymers

Aqueous Assembly and Hydrogel Rheology of Sustainable Glyoxylate-Based Copolymers

Influence of chain topology on gel formation and direct ink printing of model linear and star block copolymers with poly(ethylene oxide) and poly(ε-caprolactone) semi-crystalline blocks

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