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Title: Techniques to characterize dynamics in biomaterials microenvironments: XPCS and microrheology of alginate/PEO–PPO–PEO hydrogels

Journal Article · · Soft Matter
DOI:https://doi.org/10.1039/d0sm01628d· OSTI ID:1773139

Many recent studies have highlighted the timescale for stress relaxation of biomaterials on the microscale as an important factor in regulating a number of cell-material interactions, including cell spreading, proliferation, and differentiation. Relevant timescales on the order of 0.1–100 s have been suggested by several studies. While such timescales are accessible through conventional mechanical rheology, several biomaterials have heterogeneous structures, and stress relaxation mechanisms of the bulk material may not correspond to that experienced in the cellular microenvironment. Here we employ X-ray photon correlation spectroscopy (XPCS) to explore the temperature-dependent dynamics, relaxation time, and microrheology of multicomponent hydrogels comprising of commercial poly(ethylene oxide)–poly(propylene oxide)–poly(ethylene oxide) (PEO–PPO–PEO) triblock copolymer F127 and alginate. Previous studies on this system have shown thermoreversible behavior in the bulk oscillatory shear rheology. At physiological temperatures, bulk rheology of these samples shows behavior characteristic of a soft solid, with G' > G" and no crossover between G' and G" over the measurable frequency range, indicating a relaxation time >125 s. By contrast, XPCS-based microrheology shows viscoelastic behavior at low frequencies, and XPCS-derived correlation functions show relaxation times ranging from 10–45 s on smaller length scales. Finally, we are able to use XPCS to effectively probe the viscoelasticity and relaxation behavior within the material microenvironments.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704; DMR-1905547; CBET-1903189; DGE-1922639; CHE-1609494; NIH R01GM097971; 55729-ND9; P200A160163
OSTI ID:
1773139
Alternate ID(s):
OSTI ID: 1745071
Report Number(s):
BNL-221210-2021-JAAM
Journal Information:
Soft Matter, Vol. 17, Issue 6; ISSN 1744-683X
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (19)

Local force and geometry sensing regulate cell functions journal February 2006
Large-area alginate/PEO-PPO-PEO hydrogels with thermoreversible rheology at physiological temperatures journal January 2018
The influence of substrate creep on mesenchymal stem cell behaviour and phenotype journal September 2011
Temperature‐dependent structure and compressive mechanical behavior of alginate/polyethylene oxide–poly(propylene oxide)–poly(ethylene oxide) hydrogels
  • Quah, Suan P.; Nykypanchuk, Dmytro; Bhatia, Surita R.
  • Journal of Biomedical Materials Research Part B: Applied Biomaterials, Vol. 108, Issue 3 https://doi.org/10.1002/jbm.b.34437
journal June 2019
Hydrogels with tunable stress relaxation regulate stem cell fate and activity journal November 2015
Transport of biological molecules in surfactant–alginate composite hydrogels journal November 2011
Microrheology and structure of a yield-stress polymer gel journal April 2006
Biophysically Defined and Cytocompatible Covalently Adaptable Networks as Viscoelastic 3D Cell Culture Systems journal October 2013
Effects of PEO−PPO Diblock Impurities on the Cubic Structure of Aqueous PEO−PPO−PEO Pluronics Micelles:  fcc and bcc Ordered Structures in F127 journal March 2008
Supramolecular poly(acrylic acid)/F127 hydrogel with hydration-controlled nitric oxide release for enhancing wound healing journal July 2018
Melatonin-loaded chitosan/Pluronic® F127 microspheres as in situ forming hydrogel: An innovative antimicrobial wound dressing journal October 2016
Mechanotransduction across the cell surface and through the cytoskeleton journal May 1993
XPCS: Nanoscale motion and rheology journal February 2012
Mechanical Spectroscopy and Relaxometry on Alginate Hydrogels: A Comparative Analysis for Structural Characterization and Network Mesh Size Determination journal April 2011
Micellization of Poly(ethylene oxide)-Poly(propylene oxide)-Poly(ethylene oxide) Triblock Copolymers in Aqueous Solutions: Thermodynamics of Copolymer Association journal April 1994
Substrate Stress-Relaxation Regulates Scaffold Remodeling and Bone Formation In Vivo journal December 2016
Alginate/PEO-PPO-PEO Composite Hydrogels with Thermally-Active Plasticity journal November 2013
Curcumin incorporated PVA-borax dual delivery hydrogels as potential wound dressing materials-Correlation between viscoelastic properties and curcumin release rate journal September 2018
Multiple Phase Transition and Scaling Law for Poly(ethylene oxide)–Poly(propylene oxide)–Poly(ethylene oxide) Triblock Copolymer in Aqueous Solution journal January 2015