3D Freeform Printing of Nanocomposite Hydrogels through in situ Precipitation in Reactive Viscous Fluid

Shengyang Chen¹, Tae-Sik Jang², Houwen Matthew Pan¹, Hyun-Do Jung², Ming Wei Sia¹, Shuying Xie¹, Yao Hang³, Seow Khoon Mark Chong¹, Dongan Wang⁴, Juha Song^1*

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¹ School of Chemical and Biomedical Engineering, Nanyang Technological University, 70 Nanyang Drive, 637457, Singapore

² Liquid Processing and Casting Technology R&D Group, Korea Institute of Industrial Technology, Incheon 406-840, Republic of Korea

³ School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225009, Jiangsu, P. R. China

⁴ Department of Biomedical Engineering, City University of Hong Kong,83 Tat Chee Avenue, Kowloon Tong, Hong Kong

IJB 2020, 6(2), 258 https://doi.org/10.18063/ijb.v6i2.258

© Invalid date by the Author(s). This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution 4.0 International License ( https://creativecommons.org/licenses/by/4.0/ )

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Abstract

Composite hydrogels have gained great attention as three-dimensional (3D) printing biomaterials because of their enhanced intrinsic mechanical strength and bioactivity compared to pure hydrogels. In most conventional printing methods for composite hydrogels, particles are preloaded in ink before printing, which often reduces the printability of composite ink with little mechanical improvement due to poor particle-hydrogel interaction of physical mixing. In contrast, the in situ incorporation of nanoparticles into a hydrogel during 3D printing achieves uniform distribution of particles with remarkable mechanical reinforcement, while precursors dissolved in inks do not influence the printing process. Herein, we introduced a “printing in liquid” technique coupled with a hybridization process, which allows 3D freeform printing of nanoparticle-reinforced composite hydrogels. A viscoplastic matrix for this printing system provides not only support for printed hydrogel filaments but also chemical reactants to induce various reactions in printed objects for in situ modification. Nanocomposite hydrogel scaffolds were successfully fabricated through this 3D freeform printing of hyaluronic acid (HAc)-alginate (Alg) hydrogel inks through a two-step crosslinking strategy. The first ionic crosslinking of Alg provided structural stability during printing, while the secondary crosslinking of photo-curable HAc improved the mechanical and physiological stability of the nanocomposite hydrogels. For in situ precipitation during 3D printing, phosphate ions were dissolved in the hydrogel ink and calcium ions were added to the viscoplastic matrix. The composite hydrogels demonstrated a significant improvement in mechanical strength, biostability, as well as biological performance compared to pure HAc. Moreover, the multi-material printing of composites with different calcium phosphate contents was achieved by adjusting the ionic concentration of inks. Our method greatly accelerates the 3D printing of various functional or hybridized materials with complex geometries through the design and modification of printing materials coupled with in situ post-printing functionalization and hybridization in reactive viscoplastic matrices.

Keywords

Three-dimensional freeform printing

in situ precipitation

Hydrogels

Nanocomposites

Viscous fluid matrix

Multi-materials

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