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Simulations reveal chitosan polysaccharide chains are long and rigid in acidic conditions but shorten significantly at neutral pH. This research aids understanding of chitosan behavior in aqueous environments.

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Area of Science:

  • Polymer Science
  • Computational Chemistry
  • Biophysics

Background:

  • Chitosan polysaccharides are versatile biopolymers with applications in various fields.
  • Understanding chitosan's conformational behavior in aqueous solutions is crucial for its effective utilization.
  • Previous studies have explored chitosan properties, but detailed simulation data on chain conformation under varying pH remain limited.

Purpose of the Study:

  • To simulate chitosan polysaccharides in aqueous phase under infinite dilute conditions and zero ionic strength.
  • To investigate the effect of pH on chitosan chain conformation, specifically its persistence length.
  • To validate simulation methodologies against existing experimental and computational data.

Main Methods:

  • Utilized a polarizable multiscale modeling scheme.
  • Employed a polarizable all-atom force field for solutes and a polarizable coarse-grained solvent model.
  • Derived force field parameters from quantum chemistry ab initio data.
  • Simulated chitosan monomer units, dimers, and 50-monomer length chains at three pH conditions (85% deacetylation).

Main Results:

  • Determined the persistence length of 50-monomer chitosan chains at strong acidic conditions (pH < 5) to be 24 ± 2 nm.
  • Observed a persistence length approximately one order of magnitude shorter at usual pH conditions.
  • Simulated data align with recent experimental and computational findings on chitosan.

Conclusions:

  • Chitosan chain conformation is highly pH-dependent, exhibiting significant rigidity in acidic environments.
  • The employed multiscale modeling approach accurately captures chitosan behavior in aqueous solutions.
  • Findings provide valuable insights for designing chitosan-based materials and predicting their performance in different pH conditions.