Biomedical applications of three-dimensional (3D) printing demand complex hydrogel-based constructs laden with living cells. Advanced support materials facilitate the fabrication of such constructs. This work demonstrates the versatility and utility of a gellan fluid gel as a support bath material for fabricating freeform 3D hydrogel constructs from a variety of materials. Notably, the gellan fluid gel support bath can supply sensitive biological cross-linking agents such as enzymes to printed fluid hydrogel precursors for mild covalent hydrogel cross-linking. This mild fabrication approach is suitable for fabricating cell-laden gelatin-based constructs in which mammalian cells can form intercellular contacts within hours of fabrication; cellular activity is observed over several days within printed constructs. In addition, gellan is compatible with a wide range of ionic and thermal conditions, which makes it a suitable support material for ionically cross-linked structures generated by printing alginate-based ink formulations as well as thermosensitive hydrogel constructs formed from gelatin. Ultraviolet irradiation of printed structures within the support bath is also demonstrated for photoinitiated cross-linking of acrylated ink materials. Furthermore, gellan support material performance in terms of printed filament stability and residual support material on constructs is found to be comparable and superior, respectively, to previously reported support materials.

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Tissue engineering is a rapidly growing field, which requires advanced fabrication technologies to generate cell-laden tissue analogues with a wide range of internal and external physical features including perfusable channels, cavities, custom shapes, and spatially varying material and/or cell compositions. A versatile embedded printing methodology is proposed in this work for creating custom biomedical acellular and cell-laden hydrogel constructs by utilizing a biocompatible microgel composite matrix bath. A sacrificial material is patterned within a biocompatible hydrogel precursor matrix bath using extrusion printing to create three-dimensional features; after printing, the matrix bath is cross-linked, and the sacrificial material is flushed away to create perfusable channels within the bulk composite hydrogel matrix. The composite matrix bath material consists of jammed cross-linked hydrogel microparticles (microgels) to control rheology during fabrication along with a fluid hydrogel precursor, which is cross-linked after fabrication to form the continuous phase of the composite hydrogel. For demonstration, gellan or enzymatically cross-linked gelatin microgels are utilized with a continuous gelatin hydrogel precursor solution to make the composite matrix bath herein; the composite hydrogel matrix is formed by cross-linking the continuous gelatin phase enzymatically after printing. A variety of features including discrete channels, junctions, networks, and external contours are fabricated in the proposed composite matrix bath using embedded printing. Cell-laden constructs with printed features are also evaluated; the microgel composite hydrogel matrices support cell activity, and printed channels enhance proliferation compared to solid constructs even in static culture. The proposed method can be expanded as a solid object sculpting method to sculpt external contours by printing a shell of sacrificial ink and further discarding excess composite hydrogel matrix after printing and cross-linking. While aqueous alginate solution is used as a sacrificial ink, more advanced sacrificial materials can be utilized for better printing resolution.

Freeform three-dimensional (3D) printing of functional structures from liquid hydrophobic build materials is of great significance and widely used in various fields such as soft robotics and microfluidics. In particular, a yield-stress support bath-enabled 3D-printing methodology has been emerging to fabricate complex 3D structures. Unfortunately, the reported support bath materials are either hydrophobic or not versatile enough for the printing of a wide range of hydrophobic materials. The objective of this study is to propose a fumed silica nanoparticle-based yield-stress suspension as a hydrophobic support bath to enable 3D extrusion printing of various hydrophobic ink materials in a printing-then-solidification fashion. Hydrophobic ink is freeform-deposited in a hydrophobic fumed silica-mineral oil suspension and maintains its shape during printing; it is not cured until the whole structure is complete. Various hydrophobic inks including poly­(dimethylsiloxane) (PDMS), SU-8 resin, and epoxy-based conductive ink are printed into complex 3D structures in the fumed silica-mineral oil bath and then cured using relevant cross-linking mechanisms, even at a temperature as high as 90 °C, to prove the feasibility and versatility of the proposed printing approach. In addition, the deposited feature can easily reach a much better resolution such as 30 μm for PDMS filaments due to the negligible interfacial tension effect.

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