Journal
ADVANCED SCIENCE
Volume 5, Issue 6, Pages -Publisher
WILEY
DOI: 10.1002/advs.201701010
Keywords
hydrogels; liquid-liquid phase separation; micromechanical; polypeptides; resilin
Categories
Funding
- National Institute on Deafness and Other Communication Disorders [RO1 DC011377A]
- National Science Foundation [DMR-1609544]
- National Institute of General Medical Sciences [1-P30-GM110758-01, 1-P20-RR017716]
- shared instrumentation grant from NIH-NIGMS [S10 OD016361]
- Delaware INBRE grant from NIH-NIGMS [P20 GM103446]
- EU FP7 Marie Curie Innovative Training Network Grant [607842]
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [P20GM103446] Funding Source: NIH RePORTER
- NATIONAL INSTITUTE ON DEAFNESS AND OTHER COMMUNICATION DISORDERS [R01DC011377] Funding Source: NIH RePORTER
- OFFICE OF THE DIRECTOR, NATIONAL INSTITUTES OF HEALTH [S10OD016361] Funding Source: NIH RePORTER
- Division Of Materials Research [1609544] Funding Source: National Science Foundation
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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.
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