abstract
Protein-based hydrogels have great potential to be used as bioinks for biofabrication-driven tissue regeneration strategies due to their innate bioactivity. Nevertheless, their use as bioinks in conventional 3D bioprinting is impaired due to their intrinsic low viscosity. Using embedding bioprinting, a liquid bioink is printed within a support that physically holds the patterned filament. Inspired by the recognized microencapsulation technique complex coacervation, crystal self-healing embedding bioprinting (CLADDING) is introduced based on a highly transparent crystal supporting bath. The suitability of distinct classes of gelatins is evaluated (i.e., molecular weight distribution, isoelectric point, and ionic content), as well as the formation of gelatin-gum arabic microparticles as a function of pH, temperature, solvent, and mass ratios. Characterizing and controlling this parametric window resulted in high yields of support bath with ideal self-healing properties for interaction with protein-based bioinks. This support bath achieved transparency, which boosted light permeation within the bath. Bioprinted constructs fully composed of platelet lysates encapsulating a co-culture of human mesenchymal stromal cells and endothelial cells are obtained, demonstrating a high-dense cellular network with excellent cell viability and stability over a month. CLADDING broadens the spectrum of photocrosslinkable materials with extremely low viscosity that can now be bioprinted with sensitive cells without any additional support. Crystal self-healing embedding bioprinting (CLADDING) enables the use of low viscosity protein-based hydrogels as bioinks. By printing liquid bioinks within a transparent, self-healing support bath governed by complex coacervation, CLADDING allows for the creation of stable, high-density cellular constructs with excellent viability. This method broadens the range of biomaterials and cells that can be used in 3D bioprinting. image
keywords
HYDROGELS; TEMPERATURE; COMPLEX
subject category
Chemistry; Science & Technology - Other Topics; Materials Science
authors
Decarli, MC; Ferreira, HP; Sobreiro-Almeida, R; Teixeira, FC; Correia, TR; Babilotte, J; Olijve, J; Custodio, CA; Gonçalves, IC; Mota, C; Mano, JF; Moroni, L
our authors
acknowledgements
The authors acknowledge the support of the European Union's Horizon 2020 research and innovation program under grant agreement No 953169 (InterLynk). Helena P. Ferreira and Ines Goncalves acknowledge the financial support from Portuguese FCT for PhD grant 2020.04712.BD and contract CECINST/00091/2018/CP1500/CT0013. Rita Sobreiro-Almeida and Catarina Custodio acknowledge the Portuguese Foundation for Science and Technology for their individual grant 2022.04605.CEECIND and 2020.01647.CEECIND, respectively. The authors would also like to thank Thomas Van Gansbeke (Rousselot Biomedical) for support in the characterization of molecular weight and ion content of the gelatins used for this study.

