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Characterization of Comb-Shaped Copolymers by Multidetection SEC, DLS and SANS.

ABSTRACT: PolyCarboxylate ether-based superplasticizers (PCEs) are a type of comb-shaped copolymers used as polymeric dispersants in cementitious materials. PCEs have a high degree of dispersity, which limits the suitability of conventional characterization techniques, such as Size Exclusion Chromatography (SEC). Properties of PCEs strongly depend on their molecular structure and a comprehensive characterization is needed to fully understand the structure⁻property relationships. PCEs with well-defined molecular structures were synthesized to study their solution conformation by SEC and scattering techniques. The combined use of SEC, dynamic light scattering and small-angle neutron scattering allowed us to demonstrate the validity of a scaling law describing the radius of gyration of comb-shaped copolymers as a function of their molecular structure. Moreover, we show that the use of SEC with standard calibration, although widely spread, is not adequate for PCEs.

SUBMITTER: Gelardi G

PROVIDER: S-EPMC6432231 | biostudies-literature | 2017 Feb

REPOSITORIES: biostudies-literature

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Characterization of Comb-Shaped Copolymers by Multidetection SEC, DLS and SANS.

Gelardi Giulia G Sanson Nicolas N Nagy Gergely G Flatt Robert J RJ

Polymers 20170214 2

PolyCarboxylate ether-based superplasticizers (PCEs) are a type of comb-shaped copolymers used as polymeric dispersants in cementitious materials. PCEs have a high degree of dispersity, which limits the suitability of conventional characterization techniques, such as Size Exclusion Chromatography (SEC). Properties of PCEs strongly depend on their molecular structure and a comprehensive characterization is needed to fully understand the structure⁻property relationships. PCEs with well-defined mol ...[more]

PMID: 30970739

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Project description:Conjugating antimicrobial peptides (AMPs) to nonlinear polymers is a promising strategy to overcome the translational challenges of AMPs toward treating infections caused by antibiotic-resistant bacteria. Nonlinear polymers, and therefore conjugates, can be prepared with various architectures (e.g., star-shaped, comb-like, hyperbranched, etc.), however, the effects of polymer architecture on antimicrobial performance and related properties, like size and morphology in solution and secondary structure, are not yet well-understood. Here, we compare conjugates of the human chemokine-derived AMP stapled P9 with poly(ethylene glycol) (PEG) prepared in two of the major nonlinear architectures: star-shaped and comb-like. At comparable molecular weights and compositions (peptide wt %), comb-like conjugates afford increased helicity, solubility, antimicrobial activity, and proteolytic stability compared to star-shaped analogs. We then leveraged the expansive design space of comb-like architectures to prepare conjugates with different backbone lengths and PEG side chain lengths, with shorter PEG side chains leading to increased helicity, yet potentially less shielding from proteolytic degradation and the longest backbone lengths furnishing the most potent antimicrobial activity. Both comb-like and star-shaped conjugates display high zeta potential, indicating that the cationic AMPs were accessible for electrostatic interactions with bacterial membranes. Yet, the comb-like conjugates showed a higher fraction of unimolecular structures indicative of a lower propensity for supramolecular assembly that could be encumbering the desired AMP-bacteria interactions in the star-shaped conjugates. Together, our work shows comb-like AMP-polymer conjugates to outperform analogous star-shaped conjugates, while adding design flexibility to access an expansive range of monomer chemistries, monomer distributions, and backbone lengths to modulate performance-determining properties and ultimately furnish an effective suite of AMP-polymer materials as alternatives to conventional antibiotics for combatting bacterial infections.

Dataset Information

Characterization of Comb-Shaped Copolymers by Multidetection SEC, DLS and SANS.

Publications

Characterization of Comb-Shaped Copolymers by Multidetection SEC, DLS and SANS.

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