3D printable and biocompatible PEDOT:PSS-ionic liquid colloids with high conductivity for rapid on-demand fabrication of 3D bioelectronics.

3D printing has been widely used for on-demand prototyping of complex three-dimensional structures. In biomedical applications, PEDOT:PSS has emerged as a promising material in versatile bioelectronics due to its tissue-like mechanical properties and suitable electrical properties. However, previously developed PEDOT:PSS inks have not been able to fully utilize the advantages of commercial 3D printing due to its long post treatment times, difficulty in high aspect ratio printing, and low conductivity. We propose a one-shot strategy for the fabrication of PEDOT:PSS ink that is able to simultaneously achieve on-demand biocompatibility (no post treatment), structural integrity during 3D printing for tall three-dimensional structures, and high conductivity for rapid-prototyping. By using ionic liquid-facilitated PEDOT:PSS colloidal stacking induced by a centrifugal protocol, a viscoplastic PEDOT:PSS-ionic liquid colloidal (PILC) ink was developed. PILC inks exhibit high-aspect ratio vertical stacking, omnidirectional printability for generating suspended architectures, high conductivity (~286 S/cm), and high-resolution printing (~50 µm). We demonstrate the on-demand and versatile applicability of PILC inks through the fabrication of 3D circuit boards, on-skin physiological signal monitoring e-tattoos, and implantable bioelectronics (opto-electrocorticography recording, low voltage sciatic nerve stimulation and recording from deeper brain layers via 3D vertical spike arrays).

Viscoelastic Adhesive, Super-Conformable, and Semi-Flowable Liquid Metal Eutectogels for High-Fidelity Electrophysiological Monitoring.

Integrating gels with human skin through wearables provides unprecedented opportunities for health monitoring technology and artificial intelligence. However, most conductive hydrogels, organogels, and ionogels lack essential environmental stability, biocompatibility, and adhesion for reliable epidermal sensing. In this study, we have developed a liquid metal eutectogel simultaneously possessing superior viscoelasticity, semiflowability, and mechanical rigidity for low interfacial skin impedance, high skin adhesion, and durability. Liquid metal particles (LMPs) are employed to generate free radicals and gallium ions to accelerate the polymerization of acrylic acid monomers in a deep eutectic solvent (DES), obtaining highly viscoelastic polymer networks via physical cross-linking. In particular, graphene oxide (GO) is utilized to encapsulate the LMPs through a sonication-assisted electrostatic assembly to stabilize the LMPs in DES, which also enhances the mechanical toughness and regulates the rheological properties of the eutectogels. Our optimized semi-flowable eutectogel exhibits viscous fluid behavior at low shear rates, facilitating a highly conformable interface with hairy skin. Simultaneously, it demonstrates viscoelastic behavior at high shear rates, allowing for easy peel-off. These distinctive attributes enable the successful applications of on-skin adhesive strain sensing and high-fidelity human electrophysiological (EP) monitoring, showcasing the versatility of these ionically conductive liquid metal eutectogels in advanced personal health monitoring.