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ACS Applied Polymer Materials · 2024 · IF 4.4

Polyethylene Glycol-Based Conductive Hydrogels with Anti-Freezing, Water Retention and Self-Adhesion for Flexible Sensors

Yangengchen Zhong,Mingjie Liu,Chuyang Xiang,Yeying Lin,Youjun Guan,Kunyu Ren,Chengyun Ning,Lei Zhou,Limin Lu,Rumin Fu,Guoxin Tan

Conductive hydrogels are characterized by their extraordinary stretchability, flexibility, and biocompatibility, making them ideal materials for flexible wearable sensors. However, they often encounter challenges such as freezing and water loss, which can adversely affect their conductivity and stretching performance. In this study, we introduce a conductive hydrogel incorporating polyethylene glycol (PEG), acrylic acid (AA), acrylamide (AM), and lithium chloride (LiCl), which exhibits low-temperature tolerance, resistance to drying, self-adhesion, and mechanical robustness. The hydrogel’s excellent mechanical properties, including an elongation at break of 1120% and a toughness of 2.9 MJ m–3, are attributed to the formation of a tight polymer network between P(AA-AM) and PEG through hydrogen bonding. The multiple hydrogen bonding system between PEG and the polymer networks, combined with the hydration of LiCl and electrostatic interactions between the carboxyl group and Li+, significantly enhances the hydrogel’s freezing resistance (down to −60 °C), water retention (with only 20% water loss after 15 days), and self-adhesion (with an adhesion strength to pig skin of up to 55.08 kPa). When employed as a flexible sensor, the P(AA–AM)/PEG/LiCl hydrogel exhibited excellent sensing properties for monitoring various human motions, with an impressive gauge factor of 1.91 and electrical conductivity of 4.50 S m–1 Moreover, it maintained a high electrical conductivity (3.82 S m–1) even at −20 °C. The conductive hydrogel consistently produced stable and reliable electrical signals in response to external mechanical stimuli, making it a preferred material for human motion monitoring.

研究领域: 材料科学 · 生物医学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Stretchable and self-healing carboxymethyl cellulose/polyacrylic acid conductive hydrogels for monitoring human motions and electrophysiological signals

Xiong Liu,Lizhi Chen,Ayixianguli Sufu,Fangfei Liu

Stretchable conductive hydrogels have attracted great attention in flexible electronics. Nevertheless, conductive hydrogels would suffer from an inevitable damage during use, significantly reducing the reliability and limiting the practicability. Herein, stretchable and self-healing conductive hydrogels are designed form carboxymethyl cellulose (CMC), polyacrylic acid (PAA), and Fe 3+ , which are applied for monitoring human motions and electrophysiological signals. The plentiful H-bonding and metal coordination endow the conductive hydrogels with good mechanical (fracture strain: 917 %; fracture stress: 202 kPa; toughness: 1.1 MJ m −3 ) and self-healing properties. After self-healing, the fracture stress is almost fully recovered, the fracture strain is restored to 72 %, and the conductivity is reestablished to 98 %. The conductive hydrogels show good fatigue resistance during cyclic tensile and compressive loading-unloading tests. Furthermore, the mechanical deformation would lead to the resistance change of the hydrogel to realize the electrical signal record. So, the hydrogel was assembled into a flexible wearable sensor that has good electrical conductivity (0.779 S m −1 ), fast responsiveness (response time: 300 ms; recovery time: 200 ms) and high sensitivity (gauge factor (GF) = 7.99, 400–650 %). This work demonstrates a simple and efficient strategy for developing stretchable and self-healing conductive hydrogels in healthcare monitoring and flexible electronics.

研究领域: 材料科学 · 生物医学工程
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CARBOHYDRATE POLYMERS · 2020 · IF 7.182

A novel xanthan gum-based conductive hydrogel with excellent mechanical, biocompatible, and self-healing performances

Dawei Hua,Shuting Gao,Mengjie Zhang,Wenjing Ma,Chaobo Huang

Tough and conductive hydrogels are promising materials for various applications. However, it remains a great challenge to develop an integrated hydrogel combining outstanding mechanical, conductive, and self-healing performances. Herein, we prepared a conductive, self-healing, and tough hydrogel by constructing synergistic multiple interaction among montmorillonite (MMT), Poly (acrylamide-co-acrylonitrile) (P(AAm-co-AN)), xanthan gum (XG) and ferric ion (Fe 3+ ). The obtained xanthan gum/montmorillonite/Poly (acrylamide-co-acrylonitrile) (XG/MMT/PAAm) hydrogels showed high strain stress (0.48 MPa) and compressive stress (5.9 MPa) as well as good shape recovery after multiple loading–unloading cycle tests. Moreover, the XG/MMT/PAAm hydrogels have distinctive features such as remarkable resistance to fatigue and harsh environments, insensitivity to notch, conductive, biocompatible, pH-dependent swelling behaviors and self-healing. Therefore, the as-fabricated hydrogel delivers a new prospect for its applications in various fields, such as flexible conductive device and tissue engineering.

研究领域: 材料科学 · 生物医学工程
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JOURNAL OF APPLIED POLYMER SCIENCE · 2024 ·Vol. 141 ·期 30 ·e55701 · IF 2.7

3D printing conductive hydrogel with low modulus and anti-swelling for customized strain sensors

Chaojie Chen,Guoqing Cui,Yuanlong Li,Li Liu,Guangfeng Wu

Developing antiswelling hydrogel that retains their low modulus and has three-dimensional (3D) printability to application in the biomedical field is a current critical issue. Here, we synthesized 3D printing ink consist of poly(acrylic acid-acrylamide-allyloxypolyethyleneglycol) (P(AA-Am-APEG)) and nanosilica (SiO 2 ) by free radical polymerization, immersed the hydrogel precursor printed by ink in ferric chloride solution to prepare a low modulus, antiswelling, and conductive hydrogel. In the physical cross-linking network, the coordination interaction and hydrogen bonds contributed to excellent mechanical properties and nSiO 2 regulated rheological behavior of ink. Especially, P(AA-Am-APEG) molecular chain was a structure containing of APEG branch chain, which could endow antiswelling (the equilibrium swelling rate was only 7% in deionized water) and low modulus (Young's modulus was less than 100 kPa) to hydrogel. The tensile stress could still maintain 90% of the original value after soaking for 24 h. In addition, the existence of iron and chloride ions provided high sensitive deformation-dependent conductivity to hydrogel. Therefore, the strategy of controlling the swelling and modulus by branch chains would expand the application of hydrogel in biosensors and other fields.

研究领域: 生物医学工程 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Preparation of stretchable and self-healable dual ionically cross-linked hydrogel based on chitosan/polyacrylic acid with anti-freezing property for multi-model flexible sensing and detection

Yongzhi Liang,Yuexin Shen,Xingyue Sun,Haiyi Liang

As a kind of promising material for flexible wearable electronics, conductive hydrogels have attracted extensive interests of researchers for their inherent merits such as superior mechanical properties, biocompatibility, and permeability. Herein, we constructed a new type of highly stretchable, anti-freezing, self-healable, and conductive hydrogel based on chitosan/polyacrylic acid. The large amount of ions inside the network had five functions for the proposed hydrogel, including excellent mechanical behaviors, high conductivity, self-recovery, self-healing and anti-freezing capability. Consequently, the proposed hydrogel possessed tunable stretchability (1190–1550%), tensile strength (0.96–2.56 MPa), toughness (5.7–14.7 MJ/m 3 ), superior self-healing property (self-healing efficiency up to 83.7%), high conductivity (4.58–5.76 S/m), and excellent anti-freezing capability. To our knowledge, the self-healable hydrogel with balanced tensile strength, toughness, conductivity, and low-temperature tolerance can hardly be achieved till now. Furthermore, the conductive hydrogels exhibited high sensitivity (gauge factor up to 10.8) in a broad strain window (0–1000%) and could detect the conventional motion signals of human body such as bending of a knuckle, swallowing, and pressure signal at both room temperature and −20 °C. Moreover, the hydrogels could also be fabricated as flexible detectors to identify different temperatures, different kinds of solutions, and different concentrations of the solution.

CAS / MDL: 7783-20-2 13520-92-8
研究领域: 材料科学 · 生物医学工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Transparent, highly stretchable, adhesive, and sensitive ionic conductive hydrogel strain sensor for human motion monitoring

Jie Ren,Meng Li,Ruirui Li,Xuemiao Wang,Yan Li,Wu Yang

Due to the flexibility, ductility and tensile properties , hydrogel is considered as promising candidates for the new generation of wearable flexible devices. However, it is still a challenge to endow multiple functions such as excellent conductivity, high stretchability, self-healing, self-adhesion, and biocompatibility in one hydrogel network. Herein, a two-step method was used to prepare multifunctional transparent tannic acid/sodium alginate/polyacrylic acid/carboxymethyl cellulose/aluminum trichloride (SA/TA/PAA/CMC/Al(III)) hydrogels with high stretchability, toughness, adhesion, and conductivity. This hydrogel can adhere to various substrates both organic and inorganic materials . The highest adhesion strength of the hydrogels to the iron sheet reaches 22.33 kPa with the fracture stress being 0.16 MPa and the toughness 1.01 MJ/m 3 . Moreover, the hydrogel exhibited repeatable and durable adhesion to human skin and could be peeled off completely without any residual, irritation or allergic reactions. Additionally, the hydrogels also have good repetitive adhesion and strain sensitivity. It was demonstrated that both large-scale and small-scale movements of the human body could be monitored by directly attached to various parts of the human body by the self-adhesion. This work provides a new prospect for the design of the biocompatible hydrogels with transparent, stretchable, self-adhesive, and strain-sensitive properties for potential applications in wearable electronic sensors.

CAS / MDL: 9004-32-4
研究领域: 材料科学 · 生物医学工程
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ACS Applied Polymer Materials · 2021 · IF 4.089

Mussel-Inspired Conductive Hydrogel with Self-Healing, Adhesive, and Antibacterial Properties for Wearable Monitoring

Xiaohui Zhang,Jingjing Wei,Shengchang Lu,He Xiao,Qingxian Miao,Min Zhang,Kai Liu,Lihui Chen,Liulian Huang,Hui Wu

Hydrogels with multifunctional properties have attracted considerable interest owing to their wide range of applications in soft robotics, wearable device development, and tissue engineering. In this study, an adhesive, self-healing, and antibacterial conductive poly(dopamine methacrylate-co-methacrylatoethyl trimethyl ammonium chloride-co-acrylic acid) (PDDA) hydrogel was prepared by the free-radical copolymerization of dopamine methacrylate (DMA), methacrylatoethyl trimethyl ammonium chloride (DMC), and acrylic acid (AA). The adhesion property of the PDDA hydrogel was explored by regulating the feeding ratios of AA, DMA, and DMC. The hydrogel with a DMA/DMC/AA molar ratio of 1:4:40 exhibited strong adhesion to various materials such as iron, wood, rubber, glass, polytetrafluoroethylene, and plastic. Meanwhile, the hydrogel showed good antibacterial properties, which had a good inhibitory effect against Escherichia coli (37%) and Staphylococcus aureus (44%). In addition, because of its non-covalent bond interactions in the cross-linking network, the hydrogel exhibited excellent self-healing property when damaged. Moreover, the excellent ductility, biocompatibility, and adhesion property of the hydrogel allow better adhesion to the skin surface and conductivity to monitor the physiological activities of the human body by means of the electrical signals recorded using the transformation of strain responses. The self-healing, adhesive, antibacterial, biocompatible, and conductive hydrogel has a wide range of applications in electronic skin and wearable devices.

CAS / MDL: 62-31-7 1330-43-4
研究领域: 材料科学 · 生物医学工程 · 软体机器人技术
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A conductive hydrogel based on nature polymer agar with self-healing ability and stretchability for flexible sensors

Zhen Nie,Kelin Peng,Lizhi Lin,Jueying Yang,Zhekun Cheng,Qiang Gan,Yu Chen,Changgen Feng

Conductive hydrogels (CHs) have drawn wide attention from the field of flexible sensor for their similarities to tissues, excellent flexibility and good electrical conductivity. However, most of the reported hydrogel-based flexible sensors display the disadvantages of poor tensile strength, low sensitivity and insufficient stability, and most of them are prepared with non-degradable synthetic polymers, which have greatly limited their application. To solve these problems, in this work, we have constructed an agar-based dynamic double cross-linked CH by the dynamic crosslinking between agar and borax via borate bonds and the hydrogen bonds between agar chains. The CH exhibits excellent electrical conductivities, tensile properties and self-healing abilities. A novel two-dimensional material, MXene nanosheet, was introduced to further improve the mechanical properties and ionic conductivity of the CH with its high ionic conductivity and ability to form hydrogen bonds with agar. The obtained Agar/Borax/MXene CH displays the excellent strength and elongation of 129 kPa and 105.1 % and the satisfying ionic conductivity of 8.14 × 10 −2 S/cm. The flexible sensor assembled with Agar/Borax hydrogel with 0.15 wt% MXene exhibits a wide strain detection range from 0 to 100 %, high sensitivity (GF≈1.520) and good stability. Our work has provided a novel strategy for the construction of green flexible sensors with good mechanical properties and high sensitivity.

CAS / MDL: 9002-18-0
研究领域: 材料科学 · 生物医学工程
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Nanomaterials · 2022 ·Vol. 12 ·期 7 ·1137 · IF 5.719

A Bilayer Skin-Inspired Hydrogel with Strong Bonding Interface

Chubin He,Xiuru Xu,Yang Lin,Yang Cui,Zhengchun Peng

Conductive hydrogels are widely used in sports monitoring, healthcare, energy storage, and other fields, due to their excellent physical and chemical properties. However, synthesizing a hydrogel with synergistically good mechanical and electrical properties is still challenging. Current fabrication strategies are mainly focused on the polymerization of hydrogels with a single component, with less emphasis on combining and matching different conductive hydrogels. Inspired by the gradient modulus structures of the human skin, we propose a bilayer structure of conductive hydrogels, composed of a spray-coated poly(3,4-dihydrothieno-1,4-dioxin): poly(styrene sulfonate) (PEDOT:PSS) as the bonding interface, a relatively low modulus hydrogel on the top, and a relatively high modulus hydrogel on the bottom. The spray-coated PEDOT:PSS constructs an interlocking interface between the top and bottom hydrogels. Compared to the single layer counterparts, both the mechanical and electrical properties were significantly improved. The as-prepared hydrogel showed outstanding stretchability (1763.85 ± 161.66%), quite high toughness (9.27 ± 0.49 MJ/m3), good tensile strength (0.92 ± 0.08 MPa), and decent elastic modulus (69.16 ± 8.02 kPa). A stretchable strain sensor based on the proposed hydrogel shows good conductivity (1.76 S/m), high sensitivity (a maximum gauge factor of 18.14), and a wide response range (0–1869%). Benefitting from the modulus matching between the two layers of the hydrogels, the interfacial interlocking network, and the patch effect of the PEDOT:PSS, the strain sensor exhibits excellent interface robustness with stable performance (>12,500 cycles). These results indicate that the proposed bilayer conductive hydrogel is a promising material for stretchable electronics, soft robots, and next-generation wearables.Keywords:conductive hydrogels;bilayer structure;interface robustness;wearable sensors

研究领域: 材料科学 · 生物医学工程
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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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EUROPEAN POLYMER JOURNAL · 2022 · IF 5.546

From carbon nanotubes to ultra-sensitive, extremely-stretchable and self-healable hydrogels

Xinyue Deng,Shuai Xie,Wentang Wang,Chunhui Luo,Faliang Luo

Bearing several merits including resemblance to tissues, tunable conductivity, and mechanical flexibility, conductive hydrogels have been widely applied in wearable sensors, implantable bioelectronics, artificial skins, etc. However, the fragile nature, lack of self-healing capability, and insufficient sensitivities at low strains of traditional conductive hydrogels cannot meet the increasing demands of flexible electronics. Here, carbon nanotubes (CNTs) were dispersed in water with the assistance of bis benzyl-modified polyethylene glycol (B-PEG 181 ), which served as additional cross-linkers to prepare hydrogel by introducing acrylamide (AM) and N , N’ -methylene bisacrylamide (MBAA). The synergy of physical entanglements and π-π interactions led to extreme stretchability (0∼132 mm/mm) and self-healable capability. In addition, the introduction of CNTs and lithium chloride endowed the hydrogel with ultra-high sensitivity (GF = 122.7, at 6.0∼8.0 mm/mm strain), superior to present sensors. Consequently, the obtained sensor could detect various human motions. It is envisioned that the remarkable performances empower the obtained gel promising applications in strain sensors, human-machine interfaces, and soft robots.

研究领域: 材料科学 · 生物医学工程
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INDUSTRIAL CROPS AND PRODUCTS · 2025 · IF 6.2

Ultra-flexible anti-freezing cellulose conductive hydrogel for energy storage and self-powered sensors

Lijia Jia,Liying Zhang,Zhenghan Cai,Feng Zhu,Biao Huang,Qilin Lu

Integrating superior flexibility, conductivity, energy harvesting and broad working temperatures into cellulose hydrogel for deformable energy storage and self-powered sensors has become urgent. Herein, an ultra-flexible anti-freezing conductive versatile hydrogel is developed via synchronously regulating polyvinyl alcohol (PVA) with cellulose nanocrystals (CNCs) and covalent organic frameworks (COFs) to form a multiple hydrogen-bonded ordered network under phytic acid (PA) crosslinking synergy. Introducing COFs into hydrogel network provides continuous protons transport channel while PA generates protons and permanently secures the hierarchical structure of hydrogel, and thus endowing the hydrogel with exceptional proton conductivity (2.46 S/m), ultra-flexibility (tensile strain of 725 %), and outstanding antifreeze conductivity (withstand −40 °C). With these attributes, the hydrogel assembled supercapacitor exhibits stable energy storage capacity (84.7 mF/cm²) and bending resilience (endure bending angles of 180°), whereas the hydrogel-based triboelectric nanogenerator (TENG) presents excellent electrical output performance. Moreover, the designed hydrogel strain sensor demonstrates high sensing sensitivity, enabling stable monitoring of various joint movements and subtle facial expressions. Overall, this study presents a promising approach for designing biomass-based versatile hydrogels with outstanding mechanical performance and energy harvesting and storage functionality for emerging applications in self-powered flexible sensors.

CAS / MDL: 124-07-2 80-41-1
研究领域: 材料科学 · 能源技术 · 生物医学工程
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