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      Compliant Iontronic Triboelectric Gels with Phase-Locked Structure Enabled by Competitive Hydrogen Bonding

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          Highlights

          • A bionic phase-locked structure-inspired iontronic triboelectric gel is proposed with good mechanical compliance for wearable haptic sensing applications.

          • Competitive hydrogen bonding systems are constructed through polymer-solvent-nonsolvent interactions, and regeneration of polymers with weak hydrogen bond donors triggers controlled phase separation.

          • Self-powered haptic skin constructed with iontronic triboelectric gel has a modulus (150.6 kPa) and stretchability (> 400%) similar to that of the human body, enabling fidelity transmission of haptic signals and precise recognition of sensing objects.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-024-01387-4.

          Abstract

          Rapid advancements in flexible electronics technology propel soft tactile sensing devices toward high-level biointegration, even attaining tactile perception capabilities surpassing human skin. However, the inherent mechanical mismatch resulting from deficient biomimetic mechanical properties of sensing materials poses a challenge to the application of wearable tactile sensing devices in human–machine interaction. Inspired by the innate biphasic structure of human subcutaneous tissue, this study discloses a skin-compliant wearable iontronic triboelectric gel via phase separation induced by competitive hydrogen bonding. Solvent-nonsolvent interactions are used to construct competitive hydrogen bonding systems to trigger phase separation, and the resulting soft-hard alternating phase-locked structure confers the iontronic triboelectric gel with Young's modulus (6.8–281.9 kPa) and high tensile properties (880%) compatible with human skin. The abundance of reactive hydroxyl groups gives the gel excellent tribopositive and self-adhesive properties (peel strength > 70 N m −1). The self-powered tactile sensing skin based on this gel maintains favorable interface and mechanical stability with the working object, which greatly ensures the high fidelity and reliability of soft tactile sensing signals. This strategy, enabling skin-compliant design and broad dynamic tunability of the mechanical properties of sensing materials, presents a universal platform for broad applications from soft robots to wearable electronics.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s40820-024-01387-4.

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          Toughening elastomers with sacrificial bonds and watching them break.

          Elastomers are widely used because of their large-strain reversible deformability. Most unfilled elastomers suffer from a poor mechanical strength, which limits their use. Using sacrificial bonds, we show how brittle, unfilled elastomers can be strongly reinforced in stiffness and toughness (up to 4 megapascals and 9 kilojoules per square meter) by introducing a variable proportion of isotropically prestretched chains that can break and dissipate energy before the material fails. Chemoluminescent cross-linking molecules, which emit light as they break, map in real time where and when many of these internal bonds break ahead of a propagating crack. The simple methodology that we use to introduce sacrificial bonds, combined with the mapping of where bonds break, has the potential to stimulate the development of new classes of unfilled tough elastomers and better molecular models of the fracture of soft materials.
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            Mechanically tunable conductive interpenetrating network hydrogels that mimic the elastic moduli of biological tissue

            Conductive and stretchable materials that match the elastic moduli of biological tissue (0.5–500 kPa) are desired for enhanced interfacial and mechanical stability. Compared with inorganic and dry polymeric conductors, hydrogels made with conducting polymers are promising soft electrode materials due to their high water content. Nevertheless, most conducting polymer-based hydrogels sacrifice electronic performance to obtain useful mechanical properties. Here we report a method that overcomes this limitation using two interpenetrating hydrogel networks, one of which is formed by the gelation of the conducting polymer PEDOT:PSS. Due to the connectivity of the PEDOT:PSS network, conductivities up to 23 S m−1 are achieved, a record for stretchable PEDOT:PSS-based hydrogels. Meanwhile, the low concentration of PEDOT:PSS enables orthogonal control over the composite mechanical properties using a secondary polymer network. We demonstrate tunability of the elastic modulus over three biologically relevant orders of magnitude without compromising stretchability ( > 100%) or conductivity ( > 10 S m −1).
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              Triboelectric nanogenerator sensors for soft robotics aiming at digital twin applications

              Designing efficient sensors for soft robotics aiming at human machine interaction remains a challenge. Here, we report a smart soft-robotic gripper system based on triboelectric nanogenerator sensors to capture the continuous motion and tactile information for soft gripper. With the special distributed electrodes, the tactile sensor can perceive the contact position and area of external stimuli. The gear-based length sensor with a stretchable strip allows the continuous detection of elongation via the sequential contact of each tooth. The triboelectric sensory information collected during the operation of soft gripper is further trained by support vector machine algorithm to identify diverse objects with an accuracy of 98.1%. Demonstration of digital twin applications, which show the object identification and duplicate robotic manipulation in virtual environment according to the real-time operation of the soft-robotic gripper system, is successfully created for virtual assembly lines and unmanned warehouse applications.
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                Author and article information

                Contributors
                nieshuangxi@gxu.edu.cn
                Journal
                Nanomicro Lett
                Nanomicro Lett
                Nano-Micro Letters
                Springer Nature Singapore (Singapore )
                2311-6706
                2150-5551
                9 April 2024
                9 April 2024
                December 2024
                : 16
                : 170
                Affiliations
                School of Light Industry and Food Engineering, Guangxi University, ( https://ror.org/02c9qn167) Nanning, 530004 People’s Republic of China
                Article
                1387
                10.1007/s40820-024-01387-4
                11003937
                38592515
                88bbe0f5-82b8-4b0f-96aa-9bea692f09ab
                © The Author(s) 2024

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 20 January 2024
                : 28 February 2024
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                © Shanghai Jiao Tong University 2024

                triboelectric nanogenerator,cellulose,triboelectric gel,self-powered sensor,energy harvesting

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