Hydrogels for osteochondral repair based on photocrosslinkable carbamate dendrimers

Lovorka Degoricija, Prashant N. Bansal, Serge H M Söntjens, Neel S. Joshi, Masaya Takahashi, Brian Snyder, Mark W. Grinstaff

Research output: Contribution to journalArticle

53 Citations (Scopus)

Abstract

First generation, photocrosslinkable dendrimers consisting of natural metabolites (i.e., succinic acid, glycerol, and β-alanine) and nonimmunogenic poly(ethylen glycol) (PEG) were synthesized divergently in high yields using ester and carbamate forming reactions. Aqueous solutions of these dendrimers were photocrosslinked with an eosin-based photoinitiator to afford hydrogels. The hydrogels displayed a range of mechanical properties based on their structure, generation size, and concentration in solution. All of the hydrogels showed minimal swelling characteristics. The dendrimer solutions were then photocrosslinked in situ in an ex vivo rabbit osteochondral defect (3 mm diameter and 10 mm depth), and the resulting hydrogels were subjected to physiologically relevant dynamic loads. Magnetic resonance imaging (MRI) showed the hydrogels to be fixated in the defect site after the repetitive loading regimen. The ([G1]-PGLBA-MA)2-PEG hydrogel was chosen for the 6 month pilot in vivo rabbit study because this hydrogel scaffold could be prepared at low polymer weight (10 wt %) and possessed the largest compressive modulus of the 10% formulations, a low swelling ratio, and contained carbamate linkages, which are more hydrolytically stable than the ester linkages. The hydrogel-treated osteochondral defects showed good attachment in the defect site and histological analysis showed the presence of collagen II and glycosaminoglycans (GAGs) in the treated defects. By contrast, the contralateral unfilled defects showed poor healing and negligible GAG or collagen II production. Good mechanical properties, low swelling, good attachment to the defect site, and positive in vivo results illustrate the potential of these dendrimer-based hydrogels as scaffolds for osteochondral defect repair.

Original languageEnglish (US)
Pages (from-to)2863-2872
Number of pages10
JournalBiomacromolecules
Volume9
Issue number10
DOIs
StatePublished - Oct 2008

Fingerprint

Dendrimers
Hydrogels
Carbamates
Repair
Defects
Hydrogel
Swelling
Glycosaminoglycans
Scaffolds
Polyethylene glycols
Collagen
Esters
Mechanical properties
Glycols
Succinic Acid
Eosine Yellowish-(YS)
Dynamic loads
Metabolites
Alanine
Magnetic resonance imaging

ASJC Scopus subject areas

  • Bioengineering
  • Materials Chemistry
  • Polymers and Plastics
  • Biomaterials

Cite this

Degoricija, L., Bansal, P. N., Söntjens, S. H. M., Joshi, N. S., Takahashi, M., Snyder, B., & Grinstaff, M. W. (2008). Hydrogels for osteochondral repair based on photocrosslinkable carbamate dendrimers. Biomacromolecules, 9(10), 2863-2872. https://doi.org/10.1021/bm800658x

Hydrogels for osteochondral repair based on photocrosslinkable carbamate dendrimers. / Degoricija, Lovorka; Bansal, Prashant N.; Söntjens, Serge H M; Joshi, Neel S.; Takahashi, Masaya; Snyder, Brian; Grinstaff, Mark W.

In: Biomacromolecules, Vol. 9, No. 10, 10.2008, p. 2863-2872.

Research output: Contribution to journalArticle

Degoricija, L, Bansal, PN, Söntjens, SHM, Joshi, NS, Takahashi, M, Snyder, B & Grinstaff, MW 2008, 'Hydrogels for osteochondral repair based on photocrosslinkable carbamate dendrimers', Biomacromolecules, vol. 9, no. 10, pp. 2863-2872. https://doi.org/10.1021/bm800658x
Degoricija, Lovorka ; Bansal, Prashant N. ; Söntjens, Serge H M ; Joshi, Neel S. ; Takahashi, Masaya ; Snyder, Brian ; Grinstaff, Mark W. / Hydrogels for osteochondral repair based on photocrosslinkable carbamate dendrimers. In: Biomacromolecules. 2008 ; Vol. 9, No. 10. pp. 2863-2872.
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