Observation of dissipating solvated protons upon hydrogel formation

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Eliane P. van Dam - , Ruhr University Bochum (Author)
  • Benedikt König - , Ruhr University Bochum (Author)
  • Sashary Ramos - , Ruhr University Bochum (Author)
  • Ellen M. Adams - , Ruhr University Bochum (Author)
  • Gerhard Schwaab - , Ruhr University Bochum (Author)
  • Martina Havenith - , Ruhr University Bochum (Author)

Abstract

Aqueous hyaluronan solutions form an elastic hydrogel within a narrow pH range, around pH 2.4, making this a model system to study the conformational changes of the hydrogen bond network upon gelation. This pH-dependent behavior allows us to probe water surrounding a biologically relevant molecule in different environments (liquid versus elastic state) which change due to an environmental stimulus. Here, we use Terahertz (THz) reflection absorption spectroscopy in attenuated total reflection (ATR) geometry as a tool to study gelation. THz spectroscopy is sensitive to changes in the hydrogen-bonded water network, and here we show that we can correlate changes in macroscopic properties to changes in the solvation of hyaluronan. Above and below the gelation pH, solvated protons are present in the solutions, however, this spectral signature is completely absent between pH 2.4-2.8, which is the pH at which hyaluronan forms a hydrogel. We propose that solvated protons are forming ion pairs with hyaluronan in this pH range. Adding urea or glucose to hyaluronan solutions changes their elasticity, in which an increase or decrease in elasticity can be linked to the formation and destruction of these ion pairs, respectively.

Details

Original languageEnglish
Pages (from-to)27893-27899
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume24
Issue number45
Publication statusPublished - 17 Oct 2022
Peer-reviewedYes
Externally publishedYes

External IDs

PubMed 36367079
ORCID /0000-0002-8120-8553/work/161409566