High-Strength, Strongly Bonded Nanocomposite Hydrogels for Cartilage Repair

Polyacrylamide-based hydrogels are widely used as potential candidates for cartilage replacement. However, their bioapplicability is sternly hampered due to their limited mechanical strength and puncture resistance. In the present work, the strength of polyacrylamide (PAM) hydrogels was increased using titanium oxide (TiO2) and carbon nanotubes (CNTs) separately and a combination of TiO2 with CNTs in a PAM matrix, which was interlinked by the bonding between nanoparticles and polymers with the deployment of density functional theory (DFT) approach. The synergistic effect and strong interfacial bonding of TiO2 and CNT nanoparticles with PAM are attributed to high compressive strength, elastic modulus (>0.43 and 2.340 MPa, respectively), and puncture resistance (estimated using the needle insertion test) for the PAM-TiO2-CNT hydrogel. The PAM-TiO2-CNT composite hydrogel revealed a significant self-healing phenomenon along with a sign toward the bioactivity and cytocompatibility by forming the apatite crystals in simulated body fluid as well as showing a cell viability of similar to 99%, respectively. Furthermore, for new insights on interfacial bonding and structural and electronic features involved in the hydrogels, DFT was used. The PAM-TiO2-CNT composite model, constructed by two interfaces (PAM-TiO2 and PAM-CNT), was stabilized by H-bonding and van der Waals-type interactions. Employing the NCI plot, HOMO-LUMO gap, and natural population analysis tools, the PAM-TiO2-CNT composite has been found to be most stable. Therefore, the prepared polyacrylamide hydrogels in combination with the TiO2 and CNT can be a remarkable nanocomposite hydrogel for cartilage repair applications.

Automated summary

Polyacrylamide-based hydrogels were strengthened using titanium oxide (TiO2) and carbon nanotubes (CNTs) alone and combined in a matrix, resulting in improved mechanical properties and puncture resistance. The synergistic effect of TiO2 and CNT nanoparticles with PAM led to high compressive strength and elastic modulus, as well as significant self-healing and cytocompatibility. The stability and structural features of the PAM-TiO2-CNT composite were analyzed using density functional theory (DFT), showing promising potential for cartilage repair applications.