Microstructured Elastomer-PEG Hydrogels via Kinetic Capture of Aqueous Liquid–Liquid Phase Separation
Journal article, 2018

Heterogeneous hydrogels with desired matrix complexity are studied for a
variety of biomimetic materials. Despite the range of such microstructured
materials described, few methods permit independent control over microstructure
and microscale mechanics by precisely controlled, single-step
processing methods. Here, a phototriggered crosslinking methodology that
traps microstructures in liquid–liquid phase-separated solutions of a highly
elastomeric resilin-like polypeptide (RLP) and poly(ethylene glycol) (PEG) is
reported. RLP-rich domains of various diameters can be trapped in a PEG
continuous phase, with the kinetics of domain maturation dependent on the
degree of acrylation. The chemical composition of both hydrogel phases over
time is assessed via in situ hyperspectral coherent Raman microscopy, with
equilibrium concentrations consistent with the compositions derived from
NMR-measured coexistence curves. Atomic force microscopy reveals that
the local mechanical properties of the two phases evolve over time, even as
the bulk modulus of the material remains constant, showing that the strategy
permits control of mechanical properties on micrometer length scales, of
relevance in generating mechanically robust materials for a range of applications.
As one example, the successful encapsulation, localization, and survival
of primary cells are demonstrated and suggest the potential application of
phase-separated RLP-PEG hydrogels in regenerative medicine applications.

micromechanical

resilin

polypeptides

liquid-liquid phase separation

hydrogels

Author

Hang Kuen Lau

University of Delaware

Alexandra Paul

Chalmers, Biology and Biological Engineering, Chemical Biology

Ishnoor Sidhu

University of Delaware

Linqing Li

University of Delaware

Chandran R. Sabanayagam

Delaware Biotechnology Institute

Sapun H. Parekh

Max Planck Society

Kristi L. Kiick

University of Delaware

Advanced Science

2198-3844 (ISSN) 21983844 (eISSN)

Vol. 5 6 1701010

Female Investigators in Nonlinear Optical Nanoscopy - FINON (FINON)

European Commission (EC) (EC/FP7/607842), 2013-10-01 -- 2017-09-30.

Roots

Basic sciences

Subject Categories

Other Biological Topics

Other Chemical Engineering

Areas of Advance

Life Science Engineering (2010-2018)

DOI

10.1002/advs.201701010

PubMed

29938180

More information

Latest update

12/5/2018