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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Skin-Inspired Packaging of Injectable Hydrogel Sensors Enabled by Photopolymerizable and Swellable Hydrogels toward Sustainable Electronics

Meijin Zhao,Wenshuai Zhang,Peipei Sun,Lei Shi,Yuhua Liu,Xingshuang Zhang,Lei Zhang,Wenjia Han,Pu Chen

Flexible hydrogel-based sensors have attracted considerable interest for their potential applications in human motion detection, physiological monitoring, and electronic skin. However, the durability of hydrogel sensors is seriously hindered due to inevitable water evaporation and the lack of reusability. Herein, inspired by the skin’s delamination structures that perform sensing and barrier functions, packaged hydrogel strain sensors (PHSSs) were fabricated by employing injectable conductive hydrogel wires as strain sensing elements and another photopolymerizable hydrogel film as an external packaging layer. Thanks to the packaging strategy, multiple properties of the high sensitivity (GF = 1.63 at a strain range of 0–100%), linear sensing property (R2 > 0.99), good transparency (∼85% transmittance), and conformal adhesion (0.24–1.53 kPa) were integrated into one PHSS, which was further demonstrated to possess the capability of detecting human motions and electrophysiological signals precisely. More importantly, the enhanced lifespan (2.5 times) was achieved as a result of water evaporation inhibition by packaging, while the swelling property of the external hydrogel film endowed the PHSS with good reusability (reused for three cycles). This study provides a new strategy for fabricating sustainable hydrogel-based electronics.

研究领域: 生物医学工程 · 柔性电子学 · 材料科学
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POLYMER BULLETIN · 2020 ·Vol. 78 ·期 8 ·4551-4568 · IF 2.014

Synthesis of pH-, thermo- and salt-responsive hydrogels containing MCM-41 as crosslinker in situ for controlled drug release

Li Yinhui,Li Pengwei,Lu Jingqiong,Zhao Yansheng

Stimuli-responsive hydrogels are attracting extensive attention in drug delivery system. Here, a novel pH, thermo and salt sensitivity of composite hydrogels was synthesized in situ from polysuccinimide modified by γ-aminopropyltriethoxysilane with mesoporous molecular sieves (MCM-41) as only crosslinking agent for controlled salicylic acid release. Morphologies and thermal behaviors of KPAsp/MCM-41 hydrogels were characterized by scanning electron microscopy and thermogravimetric analysis. Swelling dynamic behaviors, pH, thermo and salt sensitivities and drug releasing capacities of composite hydrogels were also systematically investigated. The obtained results show that multi-responsive hydrogels are very sensitive to environmental pH, external temperature and ionic valence, which indicated that the MCM-41 addition not only can ameliorate the network structure, but also can enhance the drug loading and releasing capacity. The controlled salicylic acid release rates of MCM-41/KPAsp hydrogels can reach to 33.6% and 61.2% in simulated gastric fluid (pH = 1.2) and in simulated intestinal fluid at (pH = 7.4) at 37 °C, respectively. The as-synthesized multi-responsive hydrogels reported here are promising candidates for application in targeted drug delivery system.

研究领域: 材料科学 · 药学 · 生物医学工程
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

UV-Cured Dense Double Network Hydrogel via Multiple Dynamic Crosslinking for Stable Amphibious Motion Sensing

Ruizi Wu,Tianxue Zhu,Yimeng Ni,Che Wu,Wenyi Wang,Kunyang Zhao,Jianying Huang,Yuekun Lai

Although conductive hydrogels have emerged as promising materials for developing highly flexible sensors in recent years, traditional hydrogels are prone to swelling, which significantly compromises sensor performance. To address this issue, a non-swelling hydrogel is prepared through a one-step radical polymerization of acrylic acid (AA), hydroxyethyl methacrylate (HEMA), tannic acid (TA), and quaternized chitosan (QCS) in aqueous water. The resultant poly(AA-HEMA)-QCS-TA (PAHCT) hydrogel features a highly crosslinked network, attributed to the formation of multiple hydrogen bonds among the abundant hydroxyl and carboxyl groups in AA, TA, and QCS, the electrostatic interactions between poly(AA-HEMA) and QCS, as well as polymer chain entanglements. This innovative architecture significantly enhances the anti-swelling ability of the PAHCT conductive hydrogel, achieving an equilibrium swelling ratio of 5.5% in water, along with remarkable tensile properties, reaching an elongation of 990%. Furthermore, the introduction of TA further improves the hydrogel's adhesion, ensuring its durability for long-term service. Consequently, strain sensors based on the non-swelling PAHCT hydrogel are capable of effectively monitoring human activities across various strain range and enabling reliable underwater communication. These findings open new avenues for the development of wearable sensors in amphibious environments, broadening the application scope of wearable electronics.

CAS / MDL: 7647-01-0 868-77-9
研究领域: 材料科学 · 高分子化学 · 传感器技术 · 柔性电子器件 · 可穿戴设备
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MACROMOLECULES · 2021 · IF 5.985

Modification of Hydrophobic Hydrogels into a Strongly Adhesive and Tough Hydrogel by Electrostatic Interaction

Guang Huang,Zhuofu Tang,Shuaiwei Peng,Ping Zhang,Taolin Sun,Wentao Wei,Liangpeng Zeng,Honglei Guo,Hui Guo,Guozhe Meng

Synthetic hydrogels with hydrophobic interactions, which show excellent mechanical performance and good anti-swelling ability in saltwater, have great potential in various industries, such as soft robots, 3D printing, and wearable sensors. Normally, hydrophobic molecules inside a hydrophobic hydrogel tend to aggregate to form a large hydrophobic domain, leading to a phase separation phenomenon because water is a poor solvent of the hydrophobic domain. This aggregation, however, inhibits the adhesion of the hydrophobic hydrogel to various dry materials and thus limits its application in device and sensor industries. In this study, we report the synthesis of hybrid hydrogels with ionically and hydrophobically cross-linked networks. This novel hybrid hydrogel can strongly adhere to various substrates, such as glass, polypropylene, silicone, wood, and polytetrafluoroethylene, with a maximum adhesion strength measured to be 100 kPa. Meanwhile, this hybrid hydrogel can be stretched beyond 8–10 times of its initial length. We attribute this observed strong adhesion and high toughness properties to the synergy of electrostatic interactions and hydrophobic associations. With the strong adhesion and excellent tensile performance, these hydrogels may serve as a model system to explore the strong adhesion mechanism of hydrophobic hydrogels and expand the scope of hydrogel applications.

研究领域: 材料科学 · 聚合物化学 · 软体机器人 · 生物医学工程 · 可穿戴技术
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POLYMER · 2025 · IF 4.5

Highly stretchable, self-healing, and biocompatible betaine-based hydrogels with high water absorption and mechanical resilience

Yinlei Lin,Yuhao Li,Jiashang Yin,Deqiang Liu,Guozhi Xu,Haichen Zhang,Zhipeng Yang,Huawen Hu

Double-physically crosslinked hydrogels are well-known for their exceptional self-healing and mechanical properties but often fall short in terms of biological functionality. Here, we introduce a novel betaine-based zwitterionic hydrogel designed to simultaneously enhance self-healing, mechanical strength, and biocompatibility. The hydrogel is synthesized via thermally initiated free-radical polymerization and utilizes dual physical crosslinking through hydrophobic monomer-based micelles and nanoscale Laponite XLG. The incorporation of betaine monomers further boosts the biological performance of the material. The resulting hydrogel exhibits excellent swelling behavior, achieving equilibrium within 48 h, with a water absorption capacity up to 5000 % and an equilibrium water content exceeding 98 %. Mechanically, the hydrogel exhibits a remarkable elongation at break of 1228 % under tensile testing. Furthermore, it shows exceptional self-healing properties, with fracture elongation recovery of 542.72 % after 2 h and 746.88 % after 24 h. Microscopic observations confirm near-complete healing within just 3 min. Cell viability assays reveal over 95 % cell survival in the presence of hydrogel extracts, confirming its excellent biocompatibility, high water retention, and mechanical resilience.

研究领域: 材料科学 · 高分子化学 · 生物医学工程 · 软物质物理 · 纳米技术
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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 139 ·期 38 ·e52918 · IF 3.057

Superior stretchable and tough P(AA-co-AAm)/silica hybrid hydrogels enabled by acid-mediated radiation polymerization

Yukun Tian,Yongzhi Hong,Yunlong Wang,Yuan Tian,Zhihao Wang,Meixing Ai,Jun Ma

The emerging stretchable and tough hydrogels find their extraordinary contributions in widespread use. However, the applicability of existing tough hydrogels in harsh environments like highly acidic stomachs has remained a challenge. Here, we develop superior stretchable and tough P(AA -co- AAm)/SiO 2 hybrid hydrogels through radiation-induced polymerization and crosslinking in the presence of acids. The performance of the nanocomposite gels was optimized by altering fabrication variables including acid concentration, monomer composition and absorbed dose. The mechanic tests show that the protonated hybrid hydrogels displayed a high elongation at break (1919%), fracture strength (117 kPa), and compressive strength at 50% strain (126 kPa). These values are superior to those of conventional polyelectrolyte hydrogels and expect to significantly broaden the application. The proposed strategy is quite general and offers an alternative strategy to develop tough hydrogels.

研究领域: 材料科学 · 高分子化学 · 生物医学工程
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Advanced Electronic Materials · 2025 · IF 5.3

Encapsulated Organohydrogel Couplants for Wearable Ultrasounds

Xiaoru Dong,Zhi Yang,Chaoran Xu,Jun Zhao,Juntong Zhu,Haokun Yi,Hui Xu,Zhuo Li

The couplant layer that transmits sound waves to the skin is essential for ultrasound imaging. Conventional liquid-based couplants are unsuitable for wearable detectors, while polymer-based dry couplants often suffer from high acoustic attenuation. Hydrogel-based couplants possess ideal acoustic and mechanical properties; however, water evaporation restricts their application in long-term monitoring. Current strategies to improve water retention, such as encapsulating hydrogels with elastomers, typically overlook the issue of curing shrinkage. This shrinkage induces a wrinkled interface between the elastomer and hydrogel, which can cause scattering and reflection of acoustic waves, thereby compromising ultrasound quality. To address this problem, a prefabricated hydrogel is employed as a template to mitigate the curing shrinkage at the interface. In the meantime, a large amount of glycerol is added to the template to form the organohydrogel, which reduces interactions between polymer chains, further minimizing curing shrinkage and resulting in a smooth interface. Additionally, the glycerol within the organohydrogel, combined with the external encapsulation layer, enhances long-term water retention. The results demonstrate that the prepared couplants maintain stable attenuation coefficients and produce clear imaging over 8 days.

研究领域: 生物医学工程 · 材料科学
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MOLECULES · 2023 ·Vol. 28 ·期 2 ·499 · IF 4.6

A Double-Layer Hydrogel Dressing with High Mechanical Strength and Water Resistance Used for Drug Delivery

Fangzhe Liu,Zihan Wang,Hui Guo,Haichao Li,Yulan Chen,Shuang Guan

Hydrogel dressings provide a moist wound healing environment, absorb the exudates of the wound, and have better biocompatibility than traditional dressings. However, it is still difficult to meet the needs of modern medicine due to the defects in drug burst release, weak mechanical strength, and poor water retention. To solve these problems, we developed a double-layer (DL) hydrogel based on β-cyclodextrin polymer (β-CDP), poly(vinyl alcohol) (PVA), and carboxymethyl cellulose sodium (CMC) via a layer-by-layer method. Inspired by natural coconut, this hydrogel consisted of a drug release layer (DRL) and a mechanical support layer (MSL). In our design, the introduction of β-CDP into the DRL slowed the drug release rate of the DL hydrogel. Furthermore, the mechanical strength of the hydrogel was improved by immersing the MSL in a calcium chloride/boric acid solution. Combining these two layers, the tensile strength and elongation at break of the DL hydrogel reached 1504 kPa and 400%, respectively. More interestingly, the release mechanism of DL hydrogel conformed to the diffusion–relaxation–erosion model, which was different from traditional hydrogel dressings. Therefore, the as-prepared DL structure represents a feasible solution for fabricating high-performance mechanical hydrogel dressings with sustained drug release properties, and the DL hydrogel has potential to be used for medical dressings applied in daily life.Keywords:β-cyclodextrin;hydrogel dressing;double-layer hydrogel;drug release model

研究领域: 材料科学 · 生物医学工程
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Extreme Mechanics Letters · 2021 · IF 4.567

Fatigue behaviors of physical hydrogels based on hydrogen bonds

Xueqi Zhao,Jingping Wu,Yifan Zhou,Yudong Pan,Tongqing Lu,Xiaoping Song,Jian Hu

Physical hydrogels, composed of non-covalently crosslinking three dimensional polymer networks and a large amount of water, have drawn much attention due to their excellent mechanical properties such as high toughness, self-healing, self-recovery, and shape-memory. But the fatigue behaviors of physical hydrogels, especially the role of non-covalent bonds in the fatigue process, have not been well studied. Here we study fatigue damage and fatigue fracture of two kinds of physical hydrogels based on hydrogen bonding (H-bonding): poly(vinyl alcohol)/poly(acrylic acid) (PVA/PAA) gels with weak H-bonding (weak gels) and PVA/PAA-LiCl gels with strong H-bonding (strong gels). For the fatigue damage of uncut samples, both the weak and strong gels are fatigue strengthened in small deformation by stretch-induced H-bonding rearrangement, but are fatigue damaged in large deformation by chain sliding. For the fatigue fracture of precut samples, both the weak and strong gels show no measurable fatigue threshold, but the strong gel can mitigate crack growth. These results reveal the intrinsically weak non-covalent bonds cannot effectively increase the fatigue resistance of physical hydrogels. This work provides a deep perspective for developing novel anti-fatigue hydrogels.

CAS / MDL: 328-50-7 9002-89-5
研究领域: 材料科学 · 生物材料
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Micromachines · 2017 ·Vol. 8 ·期 6 ·192 · IF 1.833

Three-Dimensional Calcium Alginate Hydrogel Assembly via TiOPc-Based Light-Induced Controllable Electrodeposition

Yang Liu,Cong Wu,Hok Sum Sam Lai,Yan Ting Liu,Wen Jung Li,Ya Jing Shen

Artificial reconstruction of three-dimensional (3D) hydrogel microstructures would greatly contribute to tissue assembly in vitro, and has been widely applied in tissue engineering and drug screening. Recent technological advances in the assembly of functional hydrogel microstructures such as microfluidic, 3D bioprinting, and micromold-based 3D hydrogel fabrication methods have enabled the formation of 3D tissue constructs. However, they still lack flexibility and high efficiency, which restrict their application in 3D tissue constructs. Alternatively, we report a feasible method for the fabrication and reconstruction of customized 3D hydrogel blocks. Arbitrary hydrogel microstructures were fabricated in situ via flexible and rapid light-addressable electrodeposition. To demonstrate the versatility of this method, the higher-order assembly of 3D hydrogel blocks was investigated using a constant direct current (DC) voltage (6 V) applied between two electrodes for 20–120 s. In addition to the plane-based two-dimensional (2D) assembly, hierarchical structures—including multi-layer 3D hydrogel structures and vessel-shaped structures—could be assembled using the proposed method. Overall, we developed a platform that enables researchers to construct complex 3D hydrogel microstructures efficiently and simply, which has the potential to facilitate research on drug screening and 3D tissue constructs.Keywords:three-dimensional (3D) hydrogel assembly;TiOPc;alginate hydrogel;light-induced electrodeposition

研究领域: 生物医学工程 · 组织工程
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Applied Sciences-Basel · 2022 ·Vol. 12 ·期 22 ·11404 · IF 2.838

An Easy-to-Prepare Conductive Hydrogel for Smart Wearable Materials Based on Acrylic Derivatives and Acrylamide

Zhixin Chen,Ke Cai,Xiang Zhang,Na Lv

Electrically conductive hydrogel materials can be used as materials for wearable sensors, which can quickly and accurately detect the activities of human joints and convert these movements into electrical signals. More specifically, they have potential for application in wearable electronic devices and electronic skins. However, a number of challenges remain regarding the preparation of conductive hydrogel materials. In this study, we synthesized the P(BHMP-AM)-Zn2+hydrogel material in situ via a one-pot method using acrylic monomer derivatives, acrylamide, and zinc ions. The resulting hydrogel exhibited a high cytocompatibility (89%), excellent cyclic tensile properties, satisfactory adhesion properties (3.4 kPa), and good electrical conductivity. Furthermore, the addition of Zn2+ions imparted antibacterial properties to the hydrogel, with sterilization rates of 65.9 and 10.9% being determined against Escherichia coli and Staphylococcus aureus, respectively. The hydrogel was able to sense the activities of joints or other parts of the human body when attached to the skin, converting these movements into electrical signals to allow the real-time monitoring of motion. This conductive hydrogel material, therefore, exhibits potential for use in wearable electronic devices and electronic skins, among other devices.Keywords:acrylic derivative;antibacterial hydrogel;conductive hydrogel;strain sensor

CAS / MDL: 5970-45-6
研究领域: 材料科学 · 生物医学工程
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MACROMOLECULAR RAPID COMMUNICATIONS · 2024 · IF 4.2

Microgel-Crosslinked Thermo-Responsive Hydrogel Actuators with High Mechanical Properties and Rapid Response

Yanyu Yang,Ying Xiao,Xiang Wu,Junjie Deng,Rufang Wei,Ashuang Liu,Haiyang Chai,Rong Wang

Smart hydrogels responsive to external stimuli are promising for various applications such as soft robotics and smart devices. High mechanical strength and fast response rate are particularly important for the construction of hydrogel actuators. Herein, tough hydrogels with rapid response rates are synthesized using vinyl-functionalized poly( N -isopropylacrylamide) (PNIPAM) microgels as macro-crosslinkers and N -isopropylacrylamide as monomers. The compression strength of the obtained PNIPAM hydrogels is up to 7.13 MPa. The response rate of the microgel-crosslinked hydrogels is significantly enhanced compared with conventional chemically crosslinked PNIPAM hydrogels. The mechanical strength and response rate of hydrogels can be adjusted by varying the proportion of monomers and crosslinkers. The lower critical solution temperature (LCST) of the PNIPAM hydrogels could be tuned by copolymerizing with ionic monomer sodium methacrylate. Thermo-responsive bilayer hydrogels are fabricated using PINPAM hydrogels with different LCSTs via a layer-by-layer method. The thermo-responsive fast swelling and shrinking properties of the two layers endow the bilayer hydrogel with anisotropic structures and asymmetric response characteristics, allowing the hydrogel to respond rapidly. The bilayer hydrogels are fabricated into clamps to grab small objects and flowers that mimicked the closure of petals, and it shows great application prospects in the field of actuators.

研究领域: 材料科学 · 软体机器人 · 智能设备
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