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International Journal of Bioprinting


                                        RESEARCH ARTICLE
                                        3D printing of mechanically tough and

                                        self-healing hydrogels with carbon
                                        nanotube fillers



                                        Soo A Kim , Yeontaek Lee , Kijun Park , Jae Park , Soohwan An , Jinseok Oh ,
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                                                                                 1,2
                                        Minkyong Kang , Yurim Lee , Yejin Jo , Seung-Woo Cho , Jungmok Seo *
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                                        1 School of Electrical and Electronic Engineering, Yonsei University, Seoul 03722, Republic of Korea
                                        2 LYNK Solutec Inc., Seoul 03722, Republic of Korea
                                        3 Department of Biotechnology, Yonsei University, Seoul 03722, Republic of Korea
                                        (This article belongs to the Special Issue: Convergence of 3D Bioprinting and Nanotechnology)
                                        Abstract
                                        Hydrogels have the potential to play a crucial role in bioelectronics, as they share
                                        many properties with human tissues. However, to effectively bridge the gap between
                                        electronics and biological systems, hydrogels must possess multiple functionalities,
                                        including  toughness, stretchability,  self-healing  ability,  three-dimensional  (3D)
                                        printability, and electrical conductivity. Fabricating such tough and self-healing
                                        materials has been reported, but it still remains a challenge to fulfill all of those
                                        features, and in particular, 3D printing of hydrogel is in the early stage of the research.
                                        In this paper, we present a 3D printable, tough, and self-healing multi-functional
                                        hydrogel in one platform made from a blend of poly(vinyl alcohol) (PVA), tannic acid
                                        (TA), and poly(acrylic acid) (PAA) hydrogel ink (PVA/TA/PAA hydrogel ink). Based on
                                        a reversible hydrogen-bond (H-bond)-based  double network, the developed 3D
            *Corresponding author:      printable hydrogel ink showed excellent printability via shear-thinning behavior,
            Jungmok Seo                 allowing high printing resolution (~100 μm) and successful fabrication of 3D-printed
            (jungmok.seo@yonsei.ac.kr)  structure by layer-by-layer printing. Moreover, the PVA/TA/PAA hydrogel ink exhibited
            Citation: Kim SA, Lee Y, Park K,    high toughness (tensile loading of up to ~45.6 kPa), stretchability (elongation of
            et al., 2023, 3D printing of   approximately 650%), tissue-like Young’s modulus (~15 kPa), and self-healing ability
            mechanically tough and self-healing   within 5 min. Furthermore, carbon nanotube (CNT) fillers were successfully added to
            hydrogels with carbon nanotube
            fillers.  Int J Bioprint, 9(5): 765.   enhance the electrical conductivity of the hydrogel. We confirmed the practicality
            https://doi.org/10.18063/ijb.765  of the hydrogel inks for bioelectronics by demonstrating biocompatibility, tissue
            Received: February 6, 2023  adhesiveness, and strain sensing ability through PVA/TA/PAA/CNT hydrogel ink.
            Accepted: April 18, 2023
            Published Online: May 31, 2023
                                        Keywords: Hydrogels; 3D Printing; Toughness; Self-healing; Nanofillers;
            Copyright: © 2023 Author(s).
            This is an Open Access article   Bioelectronics
            distributed under the terms of the
            Creative Commons Attribution
            License, permitting distribution,
            and reproduction in any medium,   1. Introduction
            provided the original work is
            properly cited.             Bioelectronics are functional devices that integrate biomolecules and electronic
            Publisher’s Note: Whioce    elements to measure biosignals from various parts of the human body, including the
            Publishing remains neutral with   skin, heart, spinal cord, and brain [1,2] . Thus, they are at the core of emerging applications
            regard to jurisdictional claims in   in the medical field such as healthcare monitoring devices, drug delivery systems, and
            published maps and institutional
            affiliations.               implantable devices [3-5] . Despite the significance of bioelectronics in advanced healthcare



            Volume 9 Issue 5 (2023)                        340                         https://doi.org/10.18063/ijb.765
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