Observation of dissipating solvated protons upon hydrogel formation

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

  • Eliane P. van Dam - , Ruhr-Universität Bochum (Autor:in)
  • Benedikt König - , Ruhr-Universität Bochum (Autor:in)
  • Sashary Ramos - , Ruhr-Universität Bochum (Autor:in)
  • Ellen M. Adams - , Ruhr-Universität Bochum (Autor:in)
  • Gerhard Schwaab - , Ruhr-Universität Bochum (Autor:in)
  • Martina Havenith - , Ruhr-Universität Bochum (Autor:in)

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

OriginalspracheEnglisch
Seiten (von - bis)27893-27899
Seitenumfang7
FachzeitschriftPhysical Chemistry Chemical Physics
Jahrgang24
Ausgabenummer45
Frühes Online-Datum17 Okt. 2022
PublikationsstatusVeröffentlicht - 7 Dez. 2022
Peer-Review-StatusJa
Extern publiziertJa

Externe IDs

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