Silk Hydrogels of Tunable Structure and Viscoelastic Properties Using Different Chronological Orders of Genipin and Physical Cross-Linking

Catering the hydrogel manufacturing process toward defined viscoelastic properties for intended biomedical use is important to hydrogel scaffolding function and cell differentiation. Silk fibroin hydrogels may undergo “physical” cross-linking through β-sheet crystallization during high pressure carb...

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Published in:ACS applied materials & interfaces 2015-06, Vol.7 (22), p.12099-12108
Main Authors: Elliott, Winston H, Bonani, Walter, Maniglio, Devid, Motta, Antonella, Tan, Wei, Migliaresi, Claudio
Format: Article
Language:English
Subjects:
Carbon Dioxide - chemistry
Carbon Dioxide - pharmacology
Cell Differentiation - drug effects
Cell Engineering
Cross-Linking Reagents - chemistry
Fibroins - chemistry
Humans
Hydrogels - chemistry
Hydrogels - pharmacology
Hydrogen-Ion Concentration
Iridoids - chemistry
Protein Structure, Secondary
Silk - chemistry
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cited_by cdi_FETCH-LOGICAL-a491t-af22dd7a8343de917291841906edec6509893821ad3dd3386c06179aba4c48a33
cites cdi_FETCH-LOGICAL-a491t-af22dd7a8343de917291841906edec6509893821ad3dd3386c06179aba4c48a33
container_end_page 12108
container_issue 22
container_start_page 12099
container_title ACS applied materials & interfaces
container_volume 7
creator Elliott, Winston H
Bonani, Walter
Maniglio, Devid
Motta, Antonella
Tan, Wei
Migliaresi, Claudio
description Catering the hydrogel manufacturing process toward defined viscoelastic properties for intended biomedical use is important to hydrogel scaffolding function and cell differentiation. Silk fibroin hydrogels may undergo “physical” cross-linking through β-sheet crystallization during high pressure carbon dioxide treatment, or covalent “chemical” cross-linking by genipin. We demonstrate here that time-dependent mechanical properties are tunable in silk fibroin hydrogels by altering the chronological order of genipin cross-linking with β-sheet formation. Genipin cross-linking before β-sheet formation affects gelation mechanics through increased molecular weight, affecting gel morphology, and decreasing stiffness response. Alternately, genipin cross-linking after gelation anchored amorphous regions of the protein chain, and increasing stiffness. These differences are highlighted and validated through large amplitude oscillatory strain near physiologic levels, after incorporation of material characterization at molecular and micron length scales.
doi_str_mv 10.1021/acsami.5b02308
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source American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list)
subjects Carbon Dioxide - chemistry
Carbon Dioxide - pharmacology
Cell Differentiation - drug effects
Cell Engineering
Cross-Linking Reagents - chemistry
Fibroins - chemistry
Humans
Hydrogels - chemistry
Hydrogels - pharmacology
Hydrogen-Ion Concentration
Iridoids - chemistry
Protein Structure, Secondary
Silk - chemistry
title Silk Hydrogels of Tunable Structure and Viscoelastic Properties Using Different Chronological Orders of Genipin and Physical Cross-Linking
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