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Green Chemical Engineering · 2023 · IF 0

Bioinspired anti-freezing 3D-printable conductive hydrogel microfibers for highly-sensitive and wide-range detection of ultralow and high strains

Yi-Min Yang,Ting-Yuan Hu,Haidong Fan,Lu Shi,Shi-Yuan Zhang,Zhuang Liu,Xiao-Jie Ju,Rui Xie,Wei Wang,Liang-Yin Chu

Soft strain sensors that can transduce stretch stimuli into electrical readouts are promising as sustainable wearable electronics. However, most strain sensors cannot achieve highly-sensitive and wide-range detection of ultralow and high strains. Inspired by bamboo structures, anti-freezing microfibers made of conductive poly(vinyl alcohol) hydrogel with poly(3,4-ethylenedioxythiphene)-poly(styrenesulfonate) are developed via continuous microfluidic spinning. The microfibers provide unique bamboo-like structures with enhanced local stress to improve both their length change and resistance change upon stretching for efficient signal conversion. The microfibers allow highly-sensitive (detection limit: 0.05% strain) and wide-range (0%–400% strain) detection of ultralow and high strains, as well as features of good stretchability (485% strain) and anti-freezing property (freezing temperature: −41.1 °C), fast response (200 ms), and good repeatability. The experimental results, together with theoretical foundation analysis and finite element analysis, prove their enhanced length and resistance changes upon stretching for efficient signal conversion. By integrating microfluidic spinning with 3D-printing technique, the textiles of the microfibers can be flexibly constructed. The microfibers and their 3D-printed textiles enable high-performance monitoring of human motions including finger bending and throat vibrating during phonation. This work provides an efficient and general strategy for developing advanced conductive hydrogel microfibers as high-performance wearable strain sensors.

研究领域: 材料科学 · 生物医学工程
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CARBOHYDRATE POLYMERS · 2021 · IF 9.381

Stretchable, freezing-tolerant conductive hydrogel for wearable electronics reinforced by cellulose nanocrystals toward multiple hydrogen bonding

Huiqiang Wang,Zheng Li,Miao Zuo,Xianhai Zeng,Xing Tang,Yong Sun,Lu Lin

Conductive hydrogels have the mechanical properties and the electronic transport properties of conductive polymers, which have been widely used in the fields of energy storage and bioelectronics. However, the rigidity and brittleness of conductive polymers hinder the long-term stability of hydrogels and limit its application in new flexible electronic devices. It is a high challenging task to prepare ion-conductive hydrogels with excellent mechanical properties, anti-freeze and electrical conductivity through a simple preparation process under the action of hydrogen bonds . We present a facile strategy to prepare mechanically tough, swelling ability hydrogels reinforced by cellulose nanocrystals (CNCs). Herein, CNCs were produced by high pressure homogeneous and pretreated with deep eutectic solvent (DES). The conductivity of the hydrogel is 0.021 S/cm at room temperature . Due to the function of DMSO/H 2 O in organic solvent system, the ion-conducting hydrogel remains flexible and conductive (0.014 S/cm) at −70 °C. Hydrogel has excellent mechanical properties (stress about 1.4 MPa, strain about 1018%), excellent transparency, freezing resistance (−70 °C) and other comprehensive characteristics. The hydrogel can be assembled into a sensor for use in monitoring large and small movements of the human body, showing good responsiveness and stability.

研究领域: 材料科学 · 生物医学工程
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Polymers · 2023 ·Vol. 15 ·期 11 ·2424 · IF 5

Silver Nanoparticle-Embedded Conductive Hydrogels for Electrochemical Sensing of Hydroquinone

Tingting Xu,Huanli Gao,Orlando J. Rojas,Hongqi Dai

In this work, a conductive hydrogel was successfully synthesized, taking advantage of the high number density of active amino and hydroxyl groups in carboxymethyl chitosan and sodium carboxymethyl cellulose. These biopolymers were effectively coupled via hydrogen bonding with the nitrogen atoms of the heterocyclic rings of conductive polypyrrole. The inclusion of another biobased polymer, sodium lignosulfonate (LS), was effective to achieve highly efficient adsorption and in-situ reduction of silver ions, leading to silver nanoparticles that were embedded in the hydrogel network and used to further improve the electro-catalytic efficiency of the system. Doping of the system in the pre-gelled state led to hydrogels that could be easily attached to the electrodes. The as-prepared silver nanoparticle-embedded conductive hydrogel electrode exhibited excellent electro-catalytic activity towards hydroquinone (HQ) present in a buffer solution. At the optimum conditions, the oxidation current density peak of HQ was linear over the 0.1–100 μM concentration range, with a detection limit as low as 0.12 μM (signal-to-noise of 3). The relative standard deviation of the anodic peak current intensity was 1.37% for eight different electrodes. After one week of storage in a 0.1 M Tris-HCl buffer solution at 4 °C, the anodic peak current intensity was 93.4% of the initial current intensity. In addition, this sensor showed no interference activity, while the addition of 30 μM CC, RS, or 1 mM of different inorganic ions does not have a significant impact on the test results, enabling HQ quantification in actual water samples.Keywords:hydroquinone;silver nanoparticle-embedded;conductive hydrogel;electrochemical sensor

研究领域: 材料科学 · 分析化学 · 纳米技术
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CARBOHYDRATE POLYMERS · 2024 · IF 10.7

A triple-crosslinked, self-healing, polyvinyl alcohol/nanocellulose hydrogel for versatile sensing applications

Danning Fu,Rendang Yang,Ruibin Wang,Yang Wang,Yan Li,Huiyang Bian

Flexible conductive hydrogels (FCHs) have attracted widespread interest as versatile monoliths that can be intricately integrated with various ingredients boasting multiple functionalities. The chemicophysical properties of FCHs cover a wide range, which significantly vary in their building blocks. However, achieving both favorable mechanical strength and high conductivity simultaneously through a facile approach remains a challenge. Herein, polyvinyl alcohol, dialdehyde cellulose nanofibrils, silver nanoparticles, borax, and tannic acid are readily “one-pot” incorporated into FCHs with great tensile stress (499 kPa), tensile strain (4591 %), and compressive stress (269 kPa) due to abundant hydrogen bonding, dynamic borate-diol bonding, and intermolecular acetalization. They also exhibit desired self-healing, generalized-adhesive, and antibacterial performances. Taking advantage of these, FCHs are further employed to support an epidermal sensor, on which remarkable strain sensitivity (gauge factor = 8.22), high-pressure sensitivity (≥ 0.258 kPa −1 ), and fast response (≤ 190 ms) are recorded. Its highly adaptive mechano-electric transformability and functions can be well maintained in serving as an array unit and touch screen pen. The results well addressed in this work are anticipated to pave the universal way of engineering FCHs.

研究领域: 材料科学 · 生物医学工程
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Journal of Materials Chemistry B · 2025 · IF 5.7

A spider silk-inspired, transparent, anti-freezing ionic conductive hydrogel as a flexible sensor device

Qiuyu Xu,Mohan Hou,Lifang Wang,Xiaoyuan Liu,Xuepeng Zhang,Li Chen,Hong Qiu,Lifang Liu

As soft material ionic conductors, ionically conductive hydrogels are of great significance for the development of flexible electronics. However, it is still a great challenge to effectively design functional hydrogel structures to address various practical application scenarios (such as low temperature environments) and expand their application range (such as transparent display devices). In this paper, an anti-bacterial and ionically conductive TEMPO-oxidized cellulose nanofiber/polyvinyl alcohol/quaternary ammonium chitosan/Al3+ (CPQA–EH) hydrogel (conductivity of 7.50 ms cm−1) with high transparency (93.7%) is constructed by a simple method of solution mixing and immersion. An organic solvent is used to induce in situ phase separation and multiple interactions between molecular chains to promote crystallization. The hydrogel network structure is regulated step by step, and nanofibrils are induced in situ to form a nano-fishnet structure. The CPQA–EH ionically conductive hydrogel with a nanofibrous network exhibits excellent tensile strength (1341.86 kPa) and toughness (6992.53 kJ m−3). Meanwhile, it shows low-temperature sensing ability even at −80 °C (freezing point of −122.08 °C). The flexible sensor based on the CPQA–EH conductive hydrogel can sensitively recognize external stimuli (strain/pressure). It shows stable detection of the movement of human joints and vocalization, and the hydrogel with high transparency can also be used as a display device to recognize writing signals.

CAS / MDL: 7446-70-0 9002-89-5
研究领域: 材料科学 · 生物医学工程 · 化学工程
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CELLULOSE · 2022 ·Vol. 29 ·期 3 ·1897-1909 · IF 6.123

Stretchable, sensitive, and environment-tolerant ionic conductive organohydrogel reinforced with cellulose nanofibers for human motion monitoring

Li Miao,Yang Yutong,Yue Chengbin,Song Yongming,Manzo Maurizio,Huang Zhenhua,Cai Liping

Abstract Conductive hydrogel (CH) strain sensors have made significant progress in wearable electronic products in recent years. However, the use of aqueous solvents as the dispersion medium in CHs largely limits the scope of applications of CHs and impedes the combination of the mechanical properties and ionic conductivity, which is urgently desired to be addressed. Herein, a simple one-pot preparation of anti-freezing, anti-drying ionic CHs with high stretchability (up to 869%), toughness (6.60 MJ/m 3 ), and Young's modulus (0.56 MPa) was proposed. These CHs consist of polyvinyl alcohol, tannic acid, and sodium chloride dispersed in a solvent consisting of glycerol and cellulose nanofiber suspension. The thus-synthesized CHs exhibit good ionic conductivity (~ 0.86 S/m) and strain sensitivity (gauge factor of 8.54). The organohydrogel possesses a sensitive strain sensing capability and a wide-working temperature range (−50 °C to 60 °C), and good stability (30 d in room-temperature) to detect human movement, such as large (joint movement) and subtle movements (voice in the throat). These advantages allow organohydrogel sensors to show great potential for electronic skin, personal healthcare, and flexible wearable devices. Graphical abstract

CAS / MDL: 9002-89-5 1401-55-4
研究领域: 材料科学 · 生物医学工程 · 柔性电子
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POLYMER TESTING · 2019 · IF 2.943

Tough and conductive nanocomposite hydrogels for human motion monitoring

Yu Li,Xueru Xiong,Xianqiang Yu,Xiangbin Sun,Jia Yang,Lin Zhu,Gang Qin,Yahui Dai,Qiang Chen

Conductive hydrogels have received great attention owing to their promising applications in electrodes, supercapacitors , actuators, fuel cells, biosensors and biomedical devices and so on. However, it is still a challenge to achieve conductive hydrogels with integrated high performances, including high strength , large stretchability, high toughness, rapid self-recovery and good self-healing. In the present work, multiple physically cross-linked conductive hydrogels with integrated high performances were fabricated by in situ doping conductive PEDOT:PSS during the formation of dual physically cross-linked poly(N-hydroxyethyl acrylamide)/Laponite hydrogels. At the optimal condition, the conductive gels exhibit high tensile strength , high extensibility, high tearing energy, rapid self-recovery property without any external stimuli, high conductivity, good self-healing property, as well as sensitive strain sensing for monitoring human activities (e.g. the movements of the finger and wrist, and tiny breathing movements). Considering easy preparation and integrated high performances, our conductive gels have potential applications in wearable electronic sensors and bioelectronics.

CAS / MDL: 7727-54-0 126213-50-1
研究领域: 材料科学 · 生物医学工程
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2022 ·Vol. 33 ·期 24 ·18952-18960 · IF 2.779

Self-healing and wearable conductive hydrogels with dynamic physically crosslinked structure

Zhang Xiao Min,Yang Xiao-Li,Wang Bin

Traditional hydrogels are easily frozen or evaporated under colder or hotter temperatures, resulting in their performance degradation. In this paper, polyacrylic acid, sodium alginate, carbon nanotubes, water, and glycerol are used to synthesize self-healing, wearable, freezing resistance, and dry resistance conductive hydrogels with interpenetrating crosslinking network structure. The dynamic cross-linking network structure of the hydrogel can rapidly recover and restructure after damage. In addition, the conductive hydrogels exhibit excellent adhesion to various materials (including PTFE, iron, glass, plastic, and skin). Conductive hydrogel has excellent strain-electric sensing properties, and has high sensitivity, significant stability and repeatability. The conductive hydrogel can be used to test the movement of fingers and knee joints by strain sensing, and has excellent, sensitive, and stable resistance response. Therefore, the conductive hydrogel can be used as a wearable strain sensor for real-time detection of human joint movement. The hydrogel has better environmental adaptability and broad application prospects.

CAS / MDL: 151-21-3 110-18-9
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 45 ·e54643 · IF 3

Modified lignin-induced composite hydrogels with good mechanical properties, adhesion, and UV resistance for strain sensors

Jing Chen,Bengang Li,Xiaofeng Ma,Shuai Zhou,Qun Gu,Hua Bian,Zhenyang Luo

The flexibility and functionality of conductive hydrogels are crucial to applications under various scenarios and complex environments. Due to single functionality and weakness in mechanical properties, the application of conductive hydrogels in flexible wearable devices remains a challenge. In this study, lignin-graft-poly(acrylic acid) (LPAA) was incorporated into acrylamide (AM)/sodium chloride (NaCl) solution to fabricate composite conductive hydrogels. NaCl enhanced the conductivity of hydrogels. The hydrogen-bond crosslinking network was formed by adding LPAA into the hydrogel, which enhanced the mechanical properties of the hydrogel (the tensile strength was 96 kPa and the compressive strength was 0.54 MPa). With LPAA added, the adhesion of hydrogels was improved to 11.3 kPa on glass, 14.2 kPa on plastic, and 17.3 kPa on metal. LPAA also provided excellent UV shielding ability (99.95%) for hydrogels while maintaining good transparency. The conductive hydrogels with good sensitivity (Gauge Factor = 2.51, 100%–500%) and stability can be used as strain sensors for monitoring physical activity. It is expected to be a candidate material for future flexible wearable electronic devices.

CAS / MDL: 110-26-9
研究领域: 材料科学 · 生物医学工程
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ACS Biomaterials Science & Engineering · 2023 · IF 5.8

Fabrication of a High-Strength, Tough, Swelling-Resistant, Conductive Hydrogel via Ion Cross-Linking, Directional Freeze-Drying, and Rehydration

Jinni Luo,Huanxia Wang,Jinfei Wang,Yuan Chen,Chenglong Li,Kejun Zhong,Jie Xiang,Pengxiang Jia

Conductive hydrogels have been in huge demand in biomedical and wearable electronics. However, the application of traditional conductive hydrogels is largely limited due to their poor mechanical properties. Here, a conductive hydrogel with excellent mechanical strength and swelling resistance properties is prepared by ion cross-linking, directional freeze-drying, and rehydration. First, the acrylamide and acrylic acid are polymerized in the κ-carrageenan solution to form the hydrogel. Then, the obtained hydrogel is cross-linked with Fe3+ by soaking in ferric chloride solution. Finally, the ionic cross-linked hydrogels are reinforced by directional freeze-drying and rehydration. The resulting hydrogel has excellent tensile strength (5.67 MPa) and high toughness (7.63 MJ/m3). It is worth noting that the hydrogel also had excellent anti-swelling properties. Its mechanical strength and volume almost show no changes after soaking in deionized water for 40 days. In addition, the hydrogel exhibits good ionic conductivity (0.091 S/m), high sensitivity, and excellent stability when applied as a strain sensor. This work proposes a simple method to fabricate a conductive hydrogel with great mechanical properties and swelling resistance, which displays huge potential in varied fields.

研究领域: 生物医学工程 · 材料科学 · 可穿戴设备
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ACS Applied Polymer Materials · 2023 · IF 5

Self-Adhesive, Antifreezing, and Antidrying Conductive Glycerin/Polyacrylamide/Chitosan Quaternary Ammonium Salt Composite Hydrogel as a Flexible Strain Sensor

Song Liu,Li Wan,Feifan Hu,Zhiwei Wen,Ming Cao,Fanrong Ai

Conductive hydrogels, a type of intrinsically flexible and conductive materials, are frequently employed in soft electronics. However, because water-based hydrogels can easily freeze and dry, their long-term stability is considerably limited. Herein, a glycerol (Gly)–water binary antifreezing and antidrying hydrogel was prepared by using glycine with water as a solvent, followed by the introduction of cationic polysaccharide chitosan quaternary ammonium salts into the covalently cross-linked polyacrylamide network and addition of NaCl ions to adjust the ionic conductivity of the hydrogel. In a broad temperature range, the produced hydrogel was used for tensile and sensitive strain sensing. Because strong hydrogen bonds between Gly and water molecules are easily established, the resultant organohydrogels have good freezing and drying endurance, retaining long-term deformation even at negative temperatures. Moreover, the hydrogel exhibits good adhesion and tensile properties because of the addition of chitosan quaternary ammonium salts. At the same time, strain sensors fabricated using the hydrogel exhibit a wide operating strain range (≈1000%) and good sensitivity, stability, and repeatability, making them promising candidates for building gel-based strain sensor platforms.

CAS / MDL: 540-69-2 7647-14-5
研究领域: 材料科学 · 生物医学工程
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POLYMER · 2023 · IF 4.6

Flexible hydrogel sensor with excellent antibacterial and low temperature frost resistance

Yibo Sun,Zhe Yu,Yiyan Gao,Xiuyan Ren,Lijie Duan,Guanghui Gao

Conductive hydrogels are ideal for preparing wearable sensing devices due to their excellent stretchability and flexibility. However, most hydrogels exhibit poor frost resistance, weak water retention, and lack of biocompatibility and antibacterial properties. In this paper, polyvinyl alcohol (PVA) was used as the skeleton, water, and glycerol formed a binary solvent system, and lithium chloride and polyhexamethylene biguanide hydrochloride (PHMB) were added to the hydrogel system as functional materials . The participation of glycerol not only endowed PVA hydrogels with excellent frost resistance but also formed hydrogen bond interaction with PVA, which improved the mechanical properties of hydrogels. Meanwhile, adding PHMB made hydrogel performs excellent antibacterial properties, effectively killing E. coli (Gram-negative bacteria) and B. subtilis (Gram-positive bacteria). Furthermore, based on the introduction of LiCl, the hydrogel displayed high electrical conductivity . The prepared hydrogel sensor could repeatedly detect and distinguish between various human activities, such as walking, frowning, and speaking. Therefore, prepared multifunctional hydrogels possessed excellent application potential in the medical field, health monitoring, and other fields.

CAS / MDL: 7447-41-8 9002-89-5
研究领域: 材料科学 · 生物医学工程 · 传感技术
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