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Block Polyelectrolyte Additives That Modulate the Viscoelasticity and Enhance the Printability of Gelatin Inks at Physiological Temperatures
journal contribution
posted on 2024-02-21, 16:08 authored by Tobias Göckler, Fahed Albreiki, Defu Li, Alisa Grimm, Felix Mecklenburg, Juan Manuel Urueña, Ute Schepers, Samanvaya SrivastavaWe demonstrate the
utility of block polyelectrolyte (bPE)
additives
to enhance viscosity and resolve challenges with the three-dimensional
(3D) printability of extrusion-based biopolymer inks. The addition
of oppositely charged bPEs to solutions of photocurable gelatin methacryloyl
(GelMA) results in complexation-driven self-assembly of the bPEs,
leading to GelMA/bPE inks that are printable at physiological temperatures,
representing stark improvements over GelMA inks that suffer from low
viscosity at 37 °C, leading to low printability and poor structural
stability. The hierarchical microstructure of the self-assemblies
(either jammed micelles or 3D networks) formed by the oppositely charged
bPEs, confirmed by small-angle X-ray scattering, is attributed to
the enhancements in the shear strength and printability of the GelMA/bPE
inks. Varying bPE concentration in the inks is shown to enable tunability
of the rheological properties to meet the criteria of pre- and postextrusion
flow characteristics for 3D printing, including prominent yielding
behavior, strong shear thinning, and rapid recovery upon flow cessation.
Moreover, the bPE self-assemblies also contribute to the robustness
of the photo-cross-linked hydrogels; photo-cross-linked GelMA/bPE
hydrogels are shown to exhibit higher shear strength than photo-cross-linked
GelMA hydrogels. Last, the assessment of the printability of GelMA/bPE
inks indicates excellent printing performance, including minimal swelling
postextrusion, satisfactory retention of the filament shape upon deposition,
and satisfactory shape fidelity of the various printed constructs.
We envision this study to serve as a practical guide for the printing
of bespoke extrusion inks where bPEs are used as scaffolds and viscosity
enhancers that can be emulated in a range of photocurable precursors.
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Keywords
various printed constructsrepresenting stark improvementspostextrusion flow characteristicspoor structural stabilityeither jammed micelles37 ° cstrong shear thinningsatisfactory shape fidelitybased biopolymer inksvarying bpe concentrationphotocurable gelatin methacryloyloppositely charged bpesassemblies also contributebespoke extrusion inksblock polyelectrolyte additiveslinked gelma hydrogelsblock polyelectrolytelinked hydrogelsgelatin inksshear strengthsatisfactory retentionphotocurable precursorslinked gelmabpe hydrogelsgelma inksbpe inksviscosity enhancersrheological propertiesresolve challengesray scatteringpractical guidephysiological temperatureslow viscosityhierarchical microstructureenable tunabilityangle x
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