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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Continuous Phase Separation Induced Tough Hydrogel Fibers with Ultrahigh Conductivity for Multidimensional Soft Electronics

Zhuang Wang,Xiaoyun Xu,Ke Zhang,Renjie Tan,Shuai Zhang,Yupei Su,Jinlian Hu

Conductive hydrogel fibers exhibit great potential in soft robots, bioelectronics, and human–machine interfaces due to the unique combination of electrical conductivity, high water content, tissue-like mechanical properties, and 1D structure. Despite significant advances in hydrogel technologies, the typical conductive hydrogel fibers show low conductivity (<10 S cm −1 ), weak mechanical properties, and water stability, which makes it challenging to satisfy the requirements of practical applications. Here, a facile strategy is proposed to construct hydrogel fibers with ultrahigh conductivity and toughness by exploiting the synergistic effects of freezing-thawing, salting-out, and drying-annealing. The continuous phase separation induced by the combined processes results in hierarchical structures, promoting the formation of interconnected conductive networks and increasing the fiber's crystallinity and crystal domain size. The prepared conductive hydrogel fibers exhibited ultrahigh conductivity (≈958 S cm −1 ), excellent mechanical properties (strength (≈6.2 MPa), stretchability (>300%), and toughness (≈10 MJ m −2 )), high water content (≈75%), outstanding water stability, and fatigue resistance properties. In addition, the processibility of conductive hydrogel yarns and fabrics are demonstrated and their potential application in bioelectronics. Overall, this work presents a preparation strategy for conductive hydrogel fibers, which will facilitate the advancement of soft electronics and may inspire structural construction in other polymers.

研究领域: 材料科学 · 生物医学工程 · 软机器人技术
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Stretching-Induced 2D-to-3D Shape Transformation of an Elastic Composite for Sensitivity-Tailorable Soft Electronics

Xiangxi Cui,Min Dang,Jinqiang Jiang,Zhao-Tie Liu,Zhong-Wen Liu,Guo Li

The shapes of rubbers and elastomers are challenging to alter, and current methods relying on permanent plasticity and dynamic cross-linking strategies are usually laborious and can inevitably compromise the network elasticity. Here, we report a photoresponsive elastic composite that can be programmed into 3D shapes by first UV light irradiation and then stretching. The composite comprises ethylene propylene rubber as the elastic substrate and photoliquefiable azobenzene small molecules as the responsive filler. Upon UV light irradiation, the liquefication of the filler induces the destruction of the crystalline aggregates near the irradiated surface, and after stretching and subsequent stress release, the irradiated part bends to the irradiated side based on a gradient network orientation mechanism. The position and amplitude of bending deformation can be controlled to realize a 2D-to-3D shape transformation. We further show that the resulting 3D-shaped elastomer can integrate with silver conductive paste to develop soft conductive lines with tailorable strain-sensitive conductivities. This study may open a new door for the development of shape-tailorable elastomers and soft electronics with designable strain-sensitive conductivities.

研究领域: 材料科学 · 软体电子学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

A Universal Zwitterionic Cross-Linking Strategy for Designing Conductive Soft Electronics with Enhanced Mechanical Properties

Jinhui Luo,Kangcheng Zhao,Shuaibing Wang,Yanfang Chen,Lingbin Che,Xuanzhou Chen,Dong Zhang,Jintao Yang,Huabin Yin

Ionogels are emerging as promising electronics due to their exceptional ionic conductivity, stretchability, and high thermal stability. However, developing ionogels with enhanced mechanical properties without compromising conductivity and ion transport rates remains a significant challenge. Here, we report a zwitterionic cross-linker, 4-(2-(((2-(methacryloyloxy)ethyl)carbamoyl)oxy)ethyl)-4,14-dimethyl-8,13-dioxo-7,12-dioxa-4,9-diazapentadec-14-en-4-ium-1-propanesulfonate (MEPS) and utilized it to cross-link a variety of functional monomers, leading to the synthesis of conductive ionogels that exhibit both high mechanical strength and versatile applicability. Due to its abundant hydrogen bond donors/acceptors and zwitterionic moiety, MEPS exhibits several hundred times higher solubility in ionic liquids compared to conventional cross-linkers. As a proof-of-concept, the poly(acrylic acid-MEPS) ionogels demonstrate enhanced elongation, fracture toughness, and superior thermal stability, all while maintaining high conductivity due to the high affinity between ionic liquids and zwitterionic networks. Furthermore, MEPS-cross-linked poly(α-thioctic acid) electronics can be engineered as strain sensors, showing exceptional antifatigue properties and recyclability, remaining stable and functional over 300 consecutive cycles. This universal cross-linking strategy not only improves the overall performance of ionogels but also contributes to the development of next-generation soft electronics with enhanced functionality and durability.

研究领域: 材料科学 · 化学工程 · 软体机器人
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Highly Transparent, Stretchable, and Conducting Ionoelastomers Based on Poly(ionic liquid)s

Xiaoqing Ming,Changgeng Zhang,Junjie Cai,He Zhu,Qi Zhang,Shiping Zhu

The rapid development of soft electronics has revitalized the research of conducting elastomers. However, the design of conducting elastomers having high stretchability and good transparency still remains a considerable challenge. In this study, we develop a highly transparent, stretchable, and conducting ionoelastomer based on a poly(ionic liquid) in which cations are fixed to a stretchable elastomeric network and counter anions are mobile. The ionoelastomer solves the dilemma of simultaneous transparency and stretchability in the design of traditional conducting elastomers, possessing good transparency (96%) with an extraordinarily high stretchability, up to a limiting strain of 1460%. Moreover, this novel material is completely nonvolatile and nonhygroscopic, endowing the ionoelastomer with highly stable thermal, environmental, electrochemical, and mechanoelectrical properties. An underwater sensor based on the ionoelastomer is developed with good performance in an aqueous environment. Also, a transparent dielectric elastomer actuator (DEA) is demonstrated using the ionoelastomer. It is believed that the ionoelastomer would pave the way to develop exceptional conducting elastomers toward next-generation soft electronics.

研究领域: 材料科学 · 软电子技术 · 传感器技术
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-12 · IF 17.694

Solution-processable, soft, self-adhesive, and conductive polymer composites for soft electronics

Tan Peng,Wang Haifei,Xiao Furui,Lu Xi,Shang Wenhui,Deng Xiaobo,Song Huafeng,Xu Ziyao,Cao Junfeng,Gan Tiansheng,Wang Ben,Zhou Xuechang

Soft electronics are rising electronic technologies towards applications spanning from healthcare monitoring to medical implants. However, poor adhesion strength and significant mechanical mismatches inevitably cause the interface failure of devices. Herein we report a self-adhesive conductive polymer that possesses low modulus (56.1-401.9 kPa), high stretchability (700%), high interfacial adhesion (lap-shear strength >1.2 MPa), and high conductivity (1-37 S/cm). The self-adhesive conductive polymer is fabricated by doping the poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) composite with a supramolecular solvent (β-cyclodextrin and citric acid). We demonstrated the solution process-based fabrication of self-adhesive conductive polymer-based electrodes for various soft devices, including alternating current electroluminescent devices, electromyography monitoring, and an integrated system for the visualization of electromyography signals during muscle training with an array of alternating current electroluminescent devices. The self-adhesive conductive polymer-based electronics show promising features to further develop wearable and comfortable bioelectronic devices with the physiological electric signals of the human body readable and displayable during daily activities.

研究领域: 材料科学 · 生物医学工程 · 电子工程
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MACROMOLECULAR MATERIALS AND ENGINEERING · 2019 ·Vol. 304 ·期 12 ·1900442 · IF 3.038

High Thermal Conductivity Nanocomposites Based on Conductive Polyaniline Nanowire Arrays on Boron Nitride

Yufeng Bai,Weifang Han,Chunhua Ge,Rui Liu,Rui Zhang,Lixia Wang,Xiangdong Zhang

With the development of soft electronics, conductive composites are garnering an increasing amount of attention. The electrical conductivity, thermal conductivity, and electrical stability of conductive composites are all very important. In particular, the thermal conductivity of conductive composites is critical to the stability of their conductive properties. However, little is reported on thermal management in conductive systems. Herein, sufficiently hydroxylated boron nitride nanosheets (BN-OH)@polyaniline (PANI) composite nanosheets with a high thermal conductivity and outstanding conductance stability are reported. PANI nanowire arrays are aligned vertically on BN-OH. This well-ordered nanostructure provides the means to form a good conductive and thermally conductive path. Notably, the composite through-plane thermal conductivity is 2.1 W m −1 K −1 (≈1000% that of pure PANI) and that the resistivity of the composite is 1.38 Ω cm. Importantly, the resistivity of the composite remains unchanged after 1 h of work. The results show that this composite has prospective applications for use in soft electronics.

研究领域: 材料科学 · 电子工程
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 39 ·21093-21101 · IF 14.511

A dynamic nanoconfinement strategy towards self-healing soft electronics with super stretchability, ultrahigh strength and reliably high conductivity

Jun-Peng Wang,Chuhan Fu,Zehua Wu,Hao Lan,Siwen Cui,Tao Qi

Functions of extreme stretchability, ultrahigh tensile strength, high-level conductivity and self-healing capacity endow polymer-based soft electronics with enhanced reliability and prolonged lifespan in deformable applications. However, it is still a huge challenge to achieve such a performance portfolio in individual electronic systems because ultrahigh strength is hardly compatible with self-healing ability in polymers. Herein, a hydrogen-bonded nanoconfinement strategy is proposed to synthesize supertough self-healing polyurethane (TSPU). The hierarchical hydrogen bonds, slight covalent crosslinking and rigid nanoconfinement phases result in self-healing polymers with super stretchability and ultrahigh strength. Self-healing soft electrodes were fabricated possessing the above functions simultaneously with the TSPU polymer as the supporting layer on which a eutectic gallium–indium (EGaIn) liquid metal is spread. By means of the dynamic nanoconfinement strategy, the soft electrodes showed a break elongation of ca. 2500% and a tensile strength of ca. 50 MPa, and 200 000 times its own weight could be lifted up. Remarkably, the resistance of the soft conductor only changed a little even at 2000% strain illustrating an outstanding conductive reliability. The ultrahigh strength, extreme ductility and high reliability bring self-healing electronics to a new high level. Such self-healing soft electronic devices could find promising potential in heavy-duty deformable electronic applications.

CAS / MDL: 110-63-4 25190-06-1
研究领域: 材料科学 · 软体电子学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Instant strong adhesion of ultrafast gelling tough nanocomposite hydrogels for antifogging coatings and soft electronics

Nanbin Bao,Kun Wang,Mengxue Duan,Xuhan Gao,Yue Sun,Huan Liu,Zilian Yu,Xinmeng Zhou,Yukai Wu,Huanjun Li

Tough hydrogels capable of achieving instant and strong adhesion to diverse surfaces are highly desirable for various applications such as soft electronics and antifogging coatings. However, existing hydrogel adhesives currently suffer from several limitations including slow adhesion formation, weak bonding, and poor mechanical properties . Herein, we present that strong adhesion of tough nanocomposite hydrogels can be realized instantly by rapid copolymerization of precursor solution within seconds under ambient conditions. Such tough hydrogels possessing ultrashort gelation time were prepared based on self-catalytic Fe 3+ /tannic acid redox pairs, which could activate ammonium persulfate initiator to generate abundant sulfate radicals to trigger ultrafast copolymerization of N, N-dimethylacrylamide (DMAA) and acrylic acid (AA) in the presence of Al(OH) 3 nanoparticles . The resultant hydrogels exhibit excellent mechanical properties including tensile strength of ∼1.0 MPa and compressive strength of ∼15.0 MPa, high adhesion energy of ∼1200 J m − 2 , and good conductivity of 0.72 S/m. Benefiting from these features, the sustainable antifogging hydrogel coatings on diverse transparent substrates can be fabricated easily based on the combined advantages of ultrafast polymerization and instant strong adhesion. Furthermore, the conductive hydrogels can be assembled into flexible strain sensors to monitor various human motions and handwriting recognition. This work provides a promising strategy to design high-performance hydrogels with instant strong adhesion, antifogging properties, and strain sensing.

研究领域: 材料科学 · 生物医学工程
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MACROMOLECULAR RAPID COMMUNICATIONS · 2025 · IF 4.3

An Oriented Interpenetrating Network Structure Multi-Stimuli Responsive Hydrogel

Hui Tong,Ziwei Pan,Xie Fu,Yulong Zhou,Xia Zhang,Kun Zhang,Shuai Kang,Jinling Luo,Wenqiang Lu,Lyes Douadji

As a recent focal point of research, soft electronics encompass various factors that synergistically enhance their mechanical properties and ensure stable electrical performance. However, challenges such as immiscible conductive fillers, poor phase interfaces, and unstable conductive networks hinder the overall efficacy of these materials. To address these issues, a hydrogel featuring an oriented interpenetrating network structure (OIPN) is developed. The pyrrole monomer is in situ polymerized within the confined space of PVA macromolecular chains at low temperatures, resulting in a double network structure. Subsequently, the conductive hydrogel with an OIPN configuration is synthesized through directional freezing combined with salting out techniques. After doping phytic acid (IP6), non-covalent bonds dynamically reinforce the dual network architecture and the pathways for conductivity transfer. Due to its distinctive OIPN structure, the hydrogel containing 50% PPy and 2.3% IP6 exhibits remarkable conductivity (75 µs mm −1 ), excellent stretchability (400%), optimal multi-stimuli sensing responses (mechanical and gaseous stimuli), and outstanding device stability (over 2600 cycles at 40% strain). This multifunctional hydrogel presents a promising strategy for advancing applications in soft electronic materials.

CAS / MDL: 9002-89-5 68-04-2
研究领域: 材料科学 · 生物医学工程
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Journal of Materials Chemistry C · 2021 ·Vol. 9 ·期 28 ·8955-8965 · IF 7.393

A highly stretchable and anti-freezing silk-based conductive hydrogel for application as a self-adhesive and transparent ionotronic skin

Bohua Zhao,Qianying Chen,Gaohuan Da,Jinrong Yao,Zhengzhong Shao,Xin Chen

Soft electronic devices have rapidly developed and gained increasing attention in the past few years. Herein, a conductive silk-based hydrogel is prepared by crosslinking regenerated silk fibroin (RSF) aqueous solution with horseradish peroxidase (HRP) and adding a large amount of CaCl2 to hold water. The obtained RSF/CaCl2/HRP hydrogel is highly stretchable (breaking strain of 600% with an elastic modulus of 20 kPa) and transparent because the introduction of Ca(II) ions suppresses the formation of silk fibroin β-sheet crystals in the hydrogel. In addition, the presence of CaCl2 endows the RSF/CaCl2/HRP hydrogel with anti-drying and anti-freezing properties. The hydrogel remains soft (breaking strain of approximately 580%) and conductive (conductivity of 0.17 S m−1) at −30 °C. Moreover, the RSF/CaCl2/HRP hydrogel possesses good self-adhesive properties on different substrates, including wood, glass, metal, and plastic. The peeling strength of the hydrogel from hog skin is better than that of the commercial bandage tape. More importantly, the RSF/CaCl2/HRP hydrogel possesses both strain and temperature sensing ability. Hence, it can be assembled into a strain/temperature dual sensor. This highly stretchable, transparent, and self-adhesive strain/temperature dual sensor is a good candidate for an ionotronic skin. When tested as an ionotronic skin, the results show that this RSF-based hydrogel monitors body movements very well and can even recognize voice information from throat movements. Therefore, the proposed novel silk-based conductive hydrogel has promising potential for application in soft electronic devices.

研究领域: 材料科学 · 生物医学工程 · 软电子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2025 · IF 2.8

Hydrophobic Eutectogels for High-Humidity Environment Sensing

Xiaobo Wang,Luxin Cao,Sen Liu,Daye Guo,Kaiyuan Liu,Shuyan Yu,Yongpeng Ma,Xiaojing Zhang,Kaiqi Fan

Gels with excellent ionic conductivity and high-humidity resistance are highly desired in practical applications due to their potential to create wearable soft electronics that maintain reliable performance under humid conditions. Herein, we designed a fully hydrophobic eutectogel by one-step copolymerization of glycidyl methacrylate and 2-phenoxyethyl acrylate within a hydrophobic deep eutectic solvent (DES) composed of 1-allyl-3-methylimidazolium chloride and methyl 4-hydroxybenzoate. The optimized eutectogel exhibited exceptional moisture tolerance, featuring a water contact angle > 107° and humidity-insensitive ionic conductivity (0.10 mS·cm −1 at 90% RH). Subsequently, we fabricated a strain sensor that demonstrated stable resistance responses to multi-scale human motions, such as finger, wrist, and elbow joint bending, under both ambient and high-humidity conditions. This stability arose from the covalently crosslinked hydrophobic polymer network and non-hygroscopic DES, effectively mitigating water-induced sensing instability. The hydrophobic eutectogel sensor establishes a transformative platform for next-generation wearables in personalized healthcare and extreme-condition sensing.

研究领域: 生物医学工程 · 材料科学 · 柔性电子学 · 传感器技术 · 纳米科技 · 转化医学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Significant Roles of Ions in Enhancing and Functionalizing Anisotropic Hydrogels

Xiaoyu Wang,Chaoxu Guo,Menghan Pi,Min Li,Xiayue Yang,Honglang Lu,Wei Cui,Rong Ran

Salt ions are multifunctional in living beings, in contrast to their limited efficiency in abiotic materials. Achieving the versatility of salt ions in synthetic materials is promising yet demanding. Here, we report that multivalent metallic ions can act multiple crucial roles in a polyacrylamide/sodium alginate (PAAm/SA) composite hydrogel system, inducing a quadruple effect that toughens and functionalizes the originally weak gel. Fixation of anisotropic structures (effect I), mechanical enhancement (effect II), conductivity improvement (effect III), as well as antifreezing and moisture retention properties (effect IV) simultaneously emerge in the gel, all of which are enabled by the ion effect. The resulting tough hydrogels exhibit excellent comprehensive properties that rival existing state-of-the-art hydrogels, promising a wide range of potential applications. As proof-of-concept demonstrations, extremely durable hydrogel-based soft electronic devices are developed, which operate stably even in harsh environments. We also prove that the ion effect can be induced by other multivalent metallic ions. This work highlights the versatility of salt ions in nonliving materials, providing a simple but enlightening idea for the development of all-around soft materials.

研究领域: 材料科学 · 生物医学工程 · 化学工程
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