Mechanically resilient, injectable, and bioadhesive supramolecular gelatin hydrogels crosslinked by weak host-guest interactions assist cell infiltration and in situ tissue regeneration.
Although considered promising materials for assisting organ regeneration, few hydrogels meet the stringent requirements of clinical translation on the preparation, application, mechanical property, bioadhesion, and biocompatibility of the hydrogels. Herein, we describe a facile supramolecular approach for preparing gelatin hydrogels with a wide array of desirable properties. Briefly, we first prepare a supramolecular gelatin macromer via the efficient host-guest complexation between the aromatic residues of gelatin and free diffusing photo-crosslinkable acrylated β-cyclodextrin (β-CD) monomers. The subsequent crosslinking of the macromers produces highly resilient supramolecular gelatin hydrogels that are solely crosslinked by the weak host-guest interactions between the gelatinous aromatic residues and β-cyclodextrin (β-CD). The obtained hydrogels are capable of sustaining excessive compressive and tensile strain, and they are capable of quick self healing after mechanical disruption. These hydrogels can be injected in the gelation state through surgical needles and re-molded to the targeted geometries while protecting the encapsulated cells. Moreover, the weak host-guest crosslinking likely facilitate the infiltration and migration of cells into the hydrogels. The excess β-CDs in the hydrogels enable the hydrogel-tissue adhesion and enhance the loading and sustained delivery of hydrophobic drugs. The cell and animal studies show that such hydrogels support cell recruitment, differentiation, and bone regeneration, making them promising carrier biomaterials of therapeutic cells and drugs via minimally invasive procedures.
Division of Biomedical Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong.
Qian
Q
Feng
Division of Biomedical Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Shun Hing Institute of Advanced Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong.
Kongchang
K
Wei
Division of Biomedical Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Department of Orthopaedic and Traumatology, The Chinese University of Hong Kong, Prince of Wales Hospital, New Territories 999077, Hong Kong.
Sien
S
Lin
Department of Mechanical and Biomedical Engineering, City University of Hong Kong, Tat Chee Avenue, Kowloon 999077, Hong Kong.
Zhen
Z
Xu
Department of Orthopaedic and Traumatology, The Chinese University of Hong Kong, Prince of Wales Hospital, New Territories 999077, Hong Kong.
Yuxin
Y
Sun
Department of Mechanical and Biomedical Engineering, City University of Hong Kong, Tat Chee Avenue, Kowloon 999077, Hong Kong.
Peng
P
Shi
Department of Orthopaedic and Traumatology, The Chinese University of Hong Kong, Prince of Wales Hospital, New Territories 999077, Hong Kong.
Gang
G
Li
Division of Biomedical Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Shun Hing Institute of Advanced Engineering, The Chinese University of Hong Kong, Shatin, New Territories 999077, Hong Kong; Shenzhen Research Institue, The Chinese University of Hong Kong, Hong Kong; China Orthopedic Regenerative Medicine Group (CORMed), Hangzhou, China; Centre of Novel Biomaterials, The Chinese University of Hong Kong, Hong Kong. Electronic address: lbian@mae.cuhk.edu.hk.
Liming
L
Bian
D000179:Acrylates / Q000737:chemistry / Q000627:therapeutic use; D000818:Animals; D000893:Anti-Inflammatory Agents / Q000008:administration & dosage / Q000627:therapeutic use; D001672:Biocompatible Materials / Q000008:administration & dosage / Q000737:chemistry* / Q000627:therapeutic use; D002454:Cell Differentiation; D002460:Cell Line; D003907:Dexamethasone / Q000008:administration & dosage / Q000627:therapeutic use; D016503:Drug Delivery Systems; D005780:Gelatin / Q000008:administration & dosage / Q000737:chemistry* / Q000627:therapeutic use; D006801:Humans; D020100:Hydrogels / Q000008:administration & dosage / Q000737:chemistry* / Q000627:therapeutic use; D007267:Injections; D008297:Male; D008819:Mice, Nude; D017207:Rats, Sprague-Dawley; D013552:Swine; D013718:Tensile Strength; D000267:Tissue Adhesions / Q000628:therapy; D047392:beta-Cyclodextrins / Q000008:administration & dosage / Q000737:chemistry* / Q000627:therapeutic use
D000179:Acrylates; D000893:Anti-Inflammatory Agents; D001672:Biocompatible Materials; D020100:Hydrogels; D047392:beta-Cyclodextrins; D003907:Dexamethasone; D005780:Gelatin
Biomaterial carrier; Drug delivery; Host-guest complexation; Supramolecular hydrogel; Tissue regeneration