Block Polyelectrolyte Additives Modulate the Viscoelasticity and Enable 3D Printing of Gelatin Inks at Physiological Temperatures

23 May 2023, Version 2
This content is a preprint and has not undergone peer review at the time of posting.


We demonstrate the utility of block polyelectrolyte (bPE) additives to enhance viscosity and resolve longstanding challenges with the three-dimensional printability of extrusion-based biopolymer inks. The addition of oppositely charged bPEs into 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 three-dimensional networks) formed by the oppositely charged bPEs, as 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 post-extrusion flow characteristics for 3D bioprinting, including prominent yield stress behavior, strong shear thinning, and rapid recovery upon flow cessation. Moreover, the bPE self-assemblies also contribute to the robustness of the photocrosslinked hydrogels – photocrosslinked GelMA/bPE hydrogels are shown to exhibit higher shear strength than photocrosslinked GelMA hydrogels. We envision this study to serve as a practical guide for the bioprinting of bespoke extrusion inks where bPE are used as scaffolds and viscosity enhancers that can be emulated in a range of biopolymers and photocurable precursors.


Tissue Engineering
Additive Manufacturing
Polyelectrolyte Complexes
Self- Assembly

Supplementary materials

Supplementary Information
Supplementary figures and tables


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