Despite the development of hydrogels with high mechanical properties, insufficient adhesion between these materials and biological surfaces significantly limits their use in the biomedical field. By controlling toughening processes, we designed a composite double-network hydrogel with ~90% water content, which creates a dissipative interface and robustly adheres to soft tissues such as cartilage and meniscus. A double-network matrix composed of covalently crosslinked poly(ethylene glycol) dimethacrylate and ionically crosslinked alginate was reinforced with nano-fibrillated cellulose. No tissue surface modification was needed to obtain high adhesion properties of the developed hydrogel. Instead, mechanistic principles were used to control interfacial cracks propagation. Comparing to commercial tissue adhesives, the integration of the dissipative polymeric network on the soft tissue surfaces allowed increasing significantly the adhesion strength, such as ~130 kPa for articular cartilage. Our findings highlight the significant role of controlling hydrogel structure and dissipation processes for toughening the interface. This research provides a promising path to the development of highly adhesive hydrogels for tissues repair.

a b s t r a c tNucleus pulposus replacements have been subjected to highly controversial discussions over the last 40 years. Their use has not yet resulted in a positive outcome to treat herniated disc or degenerated disc disease. The main reason is that not a single implant or tissue replacement was able to withstand the loads within an intervertebral disc. Here, we report on the development of a photo-polymerizable poly(ethylene glycol)dimethacrylate nano-fibrillated cellulose composite hydrogel which was tuned according to native tissue properties. Using a customized minimally-invasive medical device to inject and photopolymerize the hydrogel insitu, samples were implanted through an incision of 1 mm into an intervertebral disc of a bovine organ model to evaluate their long-term performance. When implanted into the bovine disc model, the composite hydrogel implant was able to significantly re-establish disc height after surgery (p < 0.0025). The height was maintained after 0.5 million loading cycles (p < 0.025). The mechanical resistance of the novel composite hydrogel material combined with the minimally invasive implantation procedure into a bovine disc resulted in a promising functional orthopedic implant for the replacement of the nucleus pulposus.

a b s t r a c tThe application of hydrogels as load-bearing biomedical components is often limited by their mechanical properties. Often an attempt to improve a hydrogel's stiffness is accompanied by a loss of toughness and swelling properties. In this work, we show that the addition of nanofibrillated cellulose (NFC) provides a mean to tailor both the swelling and the mechanical properties of the hydrogel. Various volume fractions of NFC were added to poly(ethylene glycol) dimethacrylate (PEGDM) precursors with two different molecular weights (6 and 20 kDa). The viscosity measurements of the precursor solutions indicated that the dispersed NFCs form a network-like structure in the hydrogel precursor. Such a structure, as observed in the photo-rheology experiments, serves as a light-scattering source when the solution is illuminated by UV light, which provides a uniform polymerization of the hydrogel in three-dimension and reduces the curing time. Mechanical properties of the neat and composite hydrogels were characterized using monotonic and cyclic compression tests. NFC reinforcement increases the hydrogel's stiffness by a factor 2 and 3.5 for the PEGDM matrixes with molecular weights of 6 and 20 kDa respectively without compromising their toughness. Moreover, the desired stiffness and swelling properties can be simultaneously achieved by adapting the reinforcement concentration and the hydrogel cross-link density. The obtained composite hydrogels offer enhanced and tuneable properties and are proposed for injectable and photo-curable load-bearing implants.