TY - JOUR
T1 - Spatial-Selective Volumetric 4D Printing and Single-Photon Grafting of Biomolecules within Centimeter-Scale Hydrogels via Tomographic Manufacturing
AU - Falandt, Marc
AU - Bernal, Paulina Nuñez
AU - Dudaryeva, Oksana
AU - Florczak, Sammy
AU - Größbacher, Gabriel
AU - Schweiger, Matthias
AU - Longoni, Alessia
AU - Greant, Coralie
AU - Assunção, Marisa
AU - Nijssen, Olaf
AU - van Vlierberghe, Sandra
AU - Malda, Jos
AU - Vermonden, Tina
AU - Levato, Riccardo
N1 - Funding Information:
This project received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Grant Agreement No. 949806, VOLUME‐BIO). J.M. and R.L. acknowledge the funding from the ReumaNederland (Grant Nos. LLP‐12, LLP22 and 19‐1‐207 MINIJOINT) and the Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013). R.L. also acknowledges funding from the NWA‐Ideeëngenerator programme of the Netherlands Organization for Scientific Research (Grant No. NWA.1228.192.105). C.G. and S.v.V. acknowledge funding from the FWO EOS (Grant Agreement No. 40007548) and the FWO Hercules (Grant Agreement No. I003922N). The authors would like to acknowledge Riccardo Rizzo and Marcy Zenobi‐Wong for their advice with the gelatin characterization. The authors would like to thank Rousselot Biomedical for kindly providing the raw, low‐endotoxin gelatin materials, and Daimon J. Hall from Carbon and Neon for his support with scientific illustrations.
Funding Information:
This project received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (Grant Agreement No. 949806, VOLUME-BIO). J.M. and R.L. acknowledge the funding from the ReumaNederland (Grant Nos. LLP-12, LLP22 and 19-1-207 MINIJOINT) and the Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013). R.L. also acknowledges funding from the NWA-Ideeëngenerator programme of the Netherlands Organization for Scientific Research (Grant No. NWA.1228.192.105). C.G. and S.v.V. acknowledge funding from the FWO EOS (Grant Agreement No. 40007548) and the FWO Hercules (Grant Agreement No. I003922N). The authors would like to acknowledge Riccardo Rizzo and Marcy Zenobi-Wong for their advice with the gelatin characterization. The authors would like to thank Rousselot Biomedical for kindly providing the raw, low-endotoxin gelatin materials, and Daimon J. Hall from Carbon and Neon for his support with scientific illustrations.
Publisher Copyright:
© 2023 The Authors. Advanced Materials Technologies published by Wiley-VCH GmbH.
PY - 2023/8/11
Y1 - 2023/8/11
N2 - Conventional additive manufacturing and biofabrication techniques are unable to edit the chemicophysical properties of the printed object postprinting. Herein, a new approach is presented, leveraging light-based volumetric printing as a tool to spatially pattern any biomolecule of interest in custom-designed geometries even across large, centimeter-scale hydrogels. As biomaterial platform, a gelatin norbornene resin is developed with tunable mechanical properties suitable for tissue engineering applications. The resin can be volumetrically printed within seconds at high resolution (23.68 ± 10.75 µm). Thiol–ene click chemistry allows on-demand photografting of thiolated compounds postprinting, from small to large (bio)molecules (e.g., fluorescent dyes or growth factors). These molecules are covalently attached into printed structures using volumetric light projections, forming 3D geometries with high spatiotemporal control and ≈50 µm resolution. As a proof of concept, vascular endothelial growth factor is locally photografted into a bioprinted construct and demonstrated region-dependent enhanced adhesion and network formation of endothelial cells. This technology paves the way toward the precise spatiotemporal biofunctionalization and modification of the chemical composition of (bio)printed constructs to better guide cell behavior, build bioactive cue gradients. Moreover, it opens future possibilities for 4D printing to mimic the dynamic changes in morphogen presentation natively experienced in biological tissues.
AB - Conventional additive manufacturing and biofabrication techniques are unable to edit the chemicophysical properties of the printed object postprinting. Herein, a new approach is presented, leveraging light-based volumetric printing as a tool to spatially pattern any biomolecule of interest in custom-designed geometries even across large, centimeter-scale hydrogels. As biomaterial platform, a gelatin norbornene resin is developed with tunable mechanical properties suitable for tissue engineering applications. The resin can be volumetrically printed within seconds at high resolution (23.68 ± 10.75 µm). Thiol–ene click chemistry allows on-demand photografting of thiolated compounds postprinting, from small to large (bio)molecules (e.g., fluorescent dyes or growth factors). These molecules are covalently attached into printed structures using volumetric light projections, forming 3D geometries with high spatiotemporal control and ≈50 µm resolution. As a proof of concept, vascular endothelial growth factor is locally photografted into a bioprinted construct and demonstrated region-dependent enhanced adhesion and network formation of endothelial cells. This technology paves the way toward the precise spatiotemporal biofunctionalization and modification of the chemical composition of (bio)printed constructs to better guide cell behavior, build bioactive cue gradients. Moreover, it opens future possibilities for 4D printing to mimic the dynamic changes in morphogen presentation natively experienced in biological tissues.
KW - 4D printing
KW - biofabrication
KW - light-based printing
KW - photopatterning
KW - volumetric additive manufacturing
UR - http://www.scopus.com/inward/record.url?scp=85159898084&partnerID=8YFLogxK
U2 - 10.1002/admt.202300026
DO - 10.1002/admt.202300026
M3 - Article
AN - SCOPUS:85159898084
SN - 2365-709X
VL - 8
JO - Advanced Materials Technologies
JF - Advanced Materials Technologies
IS - 15
M1 - 2300026
ER -