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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Ultra-high stretchable, self-adhesive, and self-healable luminescent organogels with excellent anti-freezing and anti-fatigue performances for wearable sensors

Zhuoyou Gao,Hongying Lv,Zhuoer Wang,Jiali Zhang,Yushu Liu,Yajie Li,Fangzheng Zuo,Hongzan Song

Ionic conductive organogels with multifunctional capabilities have emerged as promising materials for the development of flexible and wearable ionotronic devices. However, traditional conductive organogels are often hindered by inadequate mechanical properties and complex fabrication processes. Herein, we developed multifunctional stretchable organogels with micro-phase-separated structure by one-step photopolymerization of 3-dimethyl (methacryloyloxyethyl) ammonium propane sulfonate (DMAPS) and 1-vinyl-3-butylimidazolium tetrafluoroborate (VBIMBF 4 ) monomers in glycerol. The bicontinuous phase-separated structures with electrostatic interactions and hydrogen bonds endow the resulting organogels with ultra-high stretchability, strong adhesion, rapid self-healability, excellent anti-freezing and anti-fatigue properties. Additionally, due to the crosslink-enhanced emission (CEE) effect of ionic-bonding and hydrogen-mediated interactions, these organogels exhibit unique multiple photoluminescent properties. Consequently, the developed organogels serve as highly stretchable ionic conductors suitable for wearable sensors, facilitating real-time human motion detection even at extreme low temperatures (−40 °C). The innovative characteristics of these ultra-stretchable and rapidly self-healable organogels, along with their unique photoluminescent properties, present significant opportunities for applications in wearable strain sensing within challenging environmental conditions.

研究领域: 材料科学 · 生物医学工程
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Ultra-stretchable wearable strain sensors based on skin-inspired adhesive, tough and conductive hydrogels

Qin Zhang,Xin Liu,Lijie Duan,Guanghui Gao

With increasing interest and demand for wearable sensor devices, fabricating a flexible hydrogel sensor combining high toughness and adhesiveness is necessary but remains challenging. In this work, inspired by the delamination structure of skin, an ultra-stretchable wearable hydrogel strain sensor with double layers is successfully prepared via in-situ polymerization of nucleobase-driven adhesive hydrogels on the surface of conductive tough hydrogels crosslinked by hydrophobic association. The hydrogel exhibits ultra-stretchability, high mechanical strength, and robust adhesion to various solid materials as well as skin. Furthermore, the hydrogel also exhibits high strain sensitivity and stability as a flexible and wearable strain sensor to detect large-range human motions and tiny physiological signals. Notably, the adhesive layer not only ensures a robust adhesion between the sensors and skin, but also protects skin from current harm when the hydrogels contact with skin directly, because of effectively blocking the current from the conductive tough layer. It is envisioned that the skin-inspired strategy would provide novel inspiration for the development of hydrogel strain sensors.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 140 ·期 2 ·e53287 · IF 3.057

High-strength, ultrastretchable hydrophobic association hydrogel reinforced by tailored modified carboxymethyl cellulose

Min Pan,Pengtao Wang,Zhe Xu,Yu Kuai

A new pathway to construct high-strength, ultrastretchable hydrogels based on tailored modified carboxymethyl cellulose (TMCMC)and hydrophobic association(HPA) system was investigated. TMCMC was prepared from degradation of carboxymethyl cellulose (CMC)/N,N′-methylene bisacrylamide (MBA) chemical cross-linked hydrogels. The residual double bonds of TMCMC, confirmed by 1 H-NMR and FTIR analysis, reacted with acrylamide in HPA to form TMCMC/HPA hydrogels, and the homogeneous and fine spatial network structure of TMCMC/HPA hydrogel could be observed by scanning electron microscopy. Rheological analysis revealed that the coexistence of physical and chemical crosslinking in TMCMC/HPA hydrogels. Further studies showed that TMCMC/HPA hydrogel with MBA content of 0.5 wt% has outstanding mechanical properties, and its fracture stress, elongation and tensile strength reach 1.17 MPa, 3717.05% and 15.68 MJ·m −3 , respectively. Moreover, the hydrogel displayed good swelling resistance and stable strain electrical signal response.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 生物医学工程
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STAR Protocols · 2023 · IF 0

Protocol to fabricate ionic hydrogel with ultra-stretchable and fast self-healing ability in cryogenic environments

Chan Wang,Ying Liu,Zhou Li

Summary Self-healing materials exhibit irreplaceable advantages in artificial electronics given their ability to repair from accidental damage, but the self-healing ability is temperature sensitive, limiting their applications in cryogenic environments. Here, we describe steps to fabricate a versatile ionic hydrogel with fast self-healing ability, ultra-stretchability, and stable conductivity, under the temperature ranging from −80°C to 30°C. We also detail steps for characterizing the polymer structure and interactions of the ionic hydrogel, as well as the mechanical, electrical, and self-healing properties. For complete details on the use and execution of this protocol, please refer to Wang et al. (2022). 1

研究领域: 材料科学 · 生物医学工程
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Conductive Hydrogels with Ultrastretchability and Adhesiveness for Flame- and Cold-Tolerant Strain Sensors

Cuiwen Liu,Ru Zhang,Peiwen Li,Jinqing Qu,Pengjie Chao,Zongwen Mo,Tao Yang,Ning Qing,Liuyan Tang

Hydrogel strain sensors with extreme temperature tolerance have recently gained great attention. However, the sensing ability of these hydrogel strain sensors changes with temperature, resulting in the variety of output signals that causes signal distortion. In this study, double-network hydrogels comprising SiO2 nanoparticles composed of polyacrylamide and phytic acid-doped polypyrrole were prepared and applied on strain sensors with a wide sensing range, high adhesiveness, and invariable strain sensitivity under flame and cold environments. The hydrogels had stable conductivity, excellent adhesive strength of up to 79.7 kPa on various substrates, and high elongation of up to 1896% at subzero temperature and after heating. They also exhibited effective flame retardancy with low surface temperature (71.2 °C) after 1200 s of heating (200 °C) and antifreezing properties at a low temperature of −20 °C. Remarkably, even under cold temperature and heat treatment, the hydrogel-based strain sensor displayed consistent sensing behaviors in detecting human motions with a broad strain range (up to 500%) and steady gauge factor (GF, ∼2.90). Therefore, this work paves the way for the applications of hydrogel sensors in robotic skin, human–mechanical interfaces, and health monitoring devices under harsh operating environments.

研究领域: 材料科学 · 生物医学工程
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Materials Horizons · 2023 ·Vol. 10 ·期 5 ·1865-1874 · IF 13.3

Ultra-stretchable graphene aerogels at ultralow temperatures

Guohui Yang,Xiaofang Zhang,Ruijia Wang,Xu Liu,Jianming Zhang,Lu Zong,Hongsheng Yang

Graphene aerogels (GAs) possess workable deformation and sensing properties at extreme temperatures. However, their poor tensile properties have restricted their applications in stretchable electronic devices, smart soft robots, and aerospace. Herein, an ultra-stretchable and elastic graphene aerogel with record elongation from −95% to 400% was achieved by constructing a highly crimped and crosslinked graphene network using a microbubble-filled GA precursor by a simple compress-annealing process. This conductive aerogel with near zero Poisson's ratio showed rubber-like but temperature-invariant elasticity from 196.5 °C to 300 °C, and special strain insensitivity from 50% to 400% tensile strain and high sensitivity below 50% tensile strain. Therefore, it can be used as a highly stretchable but strain-insensitive conductor under extreme environments, in which these polymer-based stretchable conductive materials are not workable. Moreover, this work provides new thoughts on constructing inorganic ultra-stretchable materials.

CAS / MDL: 50-81-7
研究领域: 材料科学 · 纳米技术
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Journal of Materials Chemistry C · 2021 ·Vol. 9 ·期 47 ·17042-17049 · IF 7.393

Design and performance of an ultra-sensitive and super-stretchable hydrogel for artificial skin

Chunhui Luo,Xinyue Deng,Shuai Xie

Designing skin-comparable conductive hydrogels has attracted tremendous interest, while it remains challenging to simultaneously achieve super-extensibility and ultra-sensitivity. Herein, a novel hydrogel was successfully fabricated to tackle this problem by using acrylamide (AM), flowerlike micelles (polyethylene glycol dilaurate) and sodium chloride (NaCl) as the monomer, cross-linker and conductive filler, respectively. The synergy of micelle deformation under external loads and chain entanglement between polyethylene glycol and polyacrylamide chains endowed the gel with an ultra-stretchable property (elongation at break of 155 mm mm−1). Meanwhile, the dipole–dipole interactions between ions and polymeric chains led to an ultra-sensitive capacity (gauge factor = 54.5, tensile strain > 20 mm mm−1), superior to those of most hydrogel-based sensors. Therefore, the obtained sensor could precisely monitor various human motions, including finger bending at different angles, speaking, walking and running. Additionally, the presence of ions (Na+ and Cl−) endowed the gel with excellent anti-freezing properties (128 mm mm−1 tensile strain at −20 °C). This work sheds light on the fabrication of high-performance sensors and will broaden their applications.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2023 ·Vol. 140 ·期 10 ·e53566 · IF 3

Rapid gelation of dual physical network hydrogel with ultra-stretchable, antifreezing, moisturing for stable and sensitive response

Yuxia Zhang,Qinglin Li,Jiawen Chen,Yanyan Zheng,Xiaoyu Lu,Qinhui Chen

Dual physical network hydrogel possesses robust energy dissipation mechanism. However, the demanding conditions of the second monomer radical polymerization aren't benefit for the dispersion of conductive filler. Moreover, the stable and sensitive response under extreme environment puts forward the requirements for mechanical, antifreezing and moisture retention properties. Herein, a dual physical networks hydrogel (polyacrylic acid-chitosan-graphene/glycerol, noted as PAA-CS-G/Gly) was prepared rapidly (<0.5 h) without chemical cross-linking agents at room temperature. The rapid gelation, ionic coordination of Ag + together with certain viscosity chitosan promoted the dispersion of graphene. PAA-CS-G/Gly showed ultra-stretchable properties (~2500%), good toughness (3.11 MJ/m 3 ), breaking strength (0.27 MPa) and fatigue resistance. PAA-CS-G/Gly had good adhesion properties, outstanding tolerance for freezing (−80°C) and moisture retention. More importantly, PAA-CS-G/Gly strain sensor had excellent sensitivity (GF, up to 9.449) at 300% ~ 900% strain. It could sensitively detect human joint movements and even subtle activities such as talking and swallowing. PAA-CS-G/Gly hydrogel is expected to adhere directly to the human body for flexible monitoring of human size movement under extreme environmental conditions.

研究领域: 材料科学 · 生物医学工程
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Bioinspired Ultra-Stretchable and Highly Sensitive Structural Color Electronic Skins

Yuanyuan Shang,Chao Huang,Zhou Li,Xuemin Du

Organisms possess remarkably adaptive ability to complex environments. For example, chameleons can alter their skin color to adapt to varying environments, which has inspired significant advances in bioinspired soft electronic skins (E-skins), and their wide applications in wearable sensors, intelligent robots, and health monitoring. However, current bioinspired E-skins face challenges in ultra-stretchability, high sensitivity, and long-term stability owing to the intrinsic limitations associated with their mismatched interface between soft matrix and hard conductive fillers, hindering their practical applications. Here, it is reported that bioinspired structural color electronic skins (SC E-skins) that consist of liquid metal particles (LMPs), periodical ordered colloidal crystal arrays, and ultra-stretchable hydrogel, imparting synergistic and durable electrical–optical sensing capabilities. Such SC E-skins demonstrate outstanding performances including superior flexibility (elongation at break > 1100%), high sensitivity (gauge factor = 3.26), fast synergetic electric–optical response time (≈100 ms), outstanding durability (over 1500 cycles), and high accuracy (R 2 > 99.5%). These bioinspired SC E-skins with excellent capability of converting mechanical signals into synergetic electrical–optical outputs hold great promise for smart wearable devices, affording a new horizon in developing advanced health monitoring technologies.

CAS / MDL: 3317-61-1
研究领域: 材料科学 · 生物医学工程 · 传感器技术
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Ultrastretchable and Antifreezing Double-Cross-Linked Cellulose Ionic Hydrogels with High Strain Sensitivity under a Broad Range of Temperature

Ruiping Tong,Guangxue Chen,Danhong Pan,Junfei Tian,Haisong Qi,Ren’ai Li,Fachuang Lu,Minghui He

Stretchable and antifreezing conductive hydrogels, especially prepared from natural polymers, are beneficial for important and rapidly growing stretchable electronic devices. Unfortunately, the potential value of the pure natural polymer-based hydrogel in such applications is very limited because of its poor mechanical behavior and inevitable freeze of water-based hydrogels at subzero temperatures. Herein, we report the ultrastretchable and antifreezing double-cross-linked cellulose ionic hydrogels (DCIHs) prepared by ammonium persulfate initiating free radical polymerization of allyl cellulose and by NaCl inducing physical cross-linking. The acquired hydrogels display ultrastretchability (∼236% of tensile strain) and high compressibility (∼82% of compression strain) among pure polysaccharide-based hydrogels including cellulose, chitosan, and chitin. Simultaneously the soaking strategy in saturated NaCl solution also endows the DCIHs with excellent antifreezing properties that not only have good stretchability (strain up to ∼100%) at −24 °C but also surprisingly transform into high visual transparency under a wide range of low temperature (−30 to −16 °C). In addition, the DCIH with high reliability, response speed, as well as wide range strain sensor is also demonstrated by investigating the output electrical signals, showing the potential for applications in flexible electronics under a broad range of temperature.

研究领域: 材料科学 · 生物医学工程 · 柔性电子
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Visible-Light Transparent, Ultrastretchable, and Self-Healable Semicrystalline Fluorinated Ionogels for Underwater Strain Sensing

Jingxiao Chen,Yufeng Wang,Le Li,Yue-E Miao,Xu Zhao,Xiu-Ping Yan,Chao Zhang,Wei Feng,Tianxi Liu

The development of ultrastretchable ionogels with a combination of high transparency and unique waterproofness is central to the development of emerging skin-inspired sensors. In this study, an ultrastretchable semicrystalline fluorinated ionogel (SFIG) with visible-light transparency and underwater stability is prepared through one-pot copolymerization of acrylic acid and fluorinated acrylate monomers in a mixed solution of poly(ethylene oxide) (PEO) and fluorinated ionic liquids. Benefiting from the formation of the PEO-chain semicrystalline microstructures and the abundant noncovalent interactions (reversible hydrogen bonds and ion–dipole interactions) in an ionogel, SFIG is rendered with room-temperature stable cross-linking structures, providing high mechanical elasticity as well as high chain segment dynamics for self-healing and efficient energy absorption during the deformation. The resultant SFIG exhibits excellent stretchability (>2500%), improved mechanical toughness (7.4 MJ m–3), and room-temperature self-healability. Due to the high compatibility and abundance of hydrophobic fluorinated moieties in the ionogel, the SFIG demonstrates high visible-light transparency (>97%) and excellent waterproofness. Due to these unique advantages, the as-prepared SFIG is capable of working as an ultrastretchable ionic conductor in capacitive-type strain sensors, demonstrating excellent underwater strain-sensing performances with high sensitivity, large detecting range, and exceptional durability. This work might provide a straightforward and efficient method for obtaining waterproof ionogel elastomers for application in next-generation underwater sensors and communications.

CAS / MDL: 684-16-2
研究领域: 材料科学 · 传感器技术 · 高分子化学
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Soft Matter · 2017 ·Vol. 13 ·期 18 ·3352-3358 · IF 3.889

Super-tough, ultra-stretchable and strongly compressive hydrogels with core–shell latex particles inducing efficient aggregation of hydrophobic chains

Xiuyan Ren,Chang Huang,Lijie Duan,Baijun Liu,Lvjun Bu,Shuang Guan,Jiliang Hou,Huixuan Zhang,Guanghui Gao

Toughness, strechability and compressibility for hydrogels were ordinarily balanced for their use as mechanically responsive materials. For example, macromolecular microsphere composite hydrogels with chemical crosslinking exhibited excellent compression strength and strechability, but poor tensile stress. Here, a novel strategy for the preparation of a super-tough, ultra-stretchable and strongly compressive hydrogel was proposed by introducing core–shell latex particles (LPs) as crosslinking centers for inducing efficient aggregation of hydrophobic chains. The core–shell LPs always maintained a spherical shape due to the presence of a hard core even by an external force and the soft shell could interact with hydrophobic chains due to hydrophobic interactions. As a result, the hydrogels reinforced by core–shell LPs exhibited not only a high tensile strength of 1.8 MPa and dramatic elongation of over 20 times, but also an excellent compressive performance of 13.5 MPa at a strain of 90%. The Mullins effect was verified for the validity of core–shell LP-reinforced hydrogels by inducing aggregation of hydrophobic chains. The novel strategy strives to provide a better avenue for designing and developing a new generation of hydrophobic association tough hydrogels with excellent mechanical properties.

研究领域: 材料科学 · 生物医学工程
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