Low-field and variable-field NMR relaxation studies of H2O and D2O molecular dynamics in articular cartilage

PLoS One. 2021 Aug 25;16(8):e0256177. doi: 10.1371/journal.pone.0256177. eCollection 2021.

Abstract

Osteoarthritis (OA) as the main degenerative disease of articular cartilage in joints is accompanied by structural and compositional changes in the tissue. Degeneration is a consequence of a reduction of the amount of macromolecules, the so-called proteoglycans, and of a corresponding increase in water content, both leading to structural weakening of cartilage. NMR investigations of cartilage generally address only the relaxation properties of water. In this study, two-dimensional (T1-T2) measurements of bovine articular cartilage samples were carried out for different stages of hydration, complemented by molecular exchange with D2O and treatment by trypsin which simulates degeneration by OA. Two signal components were identified in all measurements, characterized by very different T2 which suggests liquid-like and solid-like dynamics. These measurements allow the quantification of separate hydrogen components and their assignment to defined physical pools which had been discussed repeatedly in the literature, i.e. bulk-like water and a combination of protein hydrogens and strongly bound water. The first determination of 2H relaxation dispersion in comparison to 1H dispersion suggests intramolecular interactions as the dominating source for the pronounced magnetic field dependence of the longitudinal relaxation time T1.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Cartilage, Articular / chemistry*
  • Cattle
  • Humans
  • Joints / chemistry
  • Magnetic Resonance Spectroscopy
  • Molecular Dynamics Simulation
  • Osteoarthritis / diagnosis*
  • Osteoarthritis / metabolism
  • Osteoarthritis / pathology
  • Proteoglycans / chemistry*
  • Proteoglycans / isolation & purification
  • Water / chemistry*

Substances

  • Proteoglycans
  • Water

Associated data

  • figshare/10.6084/m9.figshare.14839098

Grants and funding

This work was supported in part by the EU Horizon 2020 collaborative project IDentIFY (project number 668119) (AC,SS, CM).The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. There was no additional external funding received for this study.