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ACS Applied Polymer Materials · 2020 · IF 0

Hydrogen-Bonding Reinforced Injectable Hydrogels: Application As a Thermo-Triggered Drug Controlled-Release System

Dong Wang,Yuzheng Xia,Dong Zhang,Xiaomeng Sun,Xiaonong Chen,Susan Oliver,Shuxian Shi,Lei Lei

Most injectable hydrogels are prone to irreversible deformation or damage under sustained shear forces and exhibit low mechanical properties, which limit their practical applications in biological engineering. In this work, the first hydrogen-bonding reinforced injectable thermoresponsive hydrogel system has been fabricated through an in situ hydrazide–aldehyde cross-linking reaction between hydrazide-functionalized poly(N-isopropylacrylamide) (PNIPAM) and dialdehyde dextrin. The mechanical strength and stability of the hydrogel were reinforced by the introduction of intermolecular hydrogen-bonding from poly(N-acryloyl glycinamide) (PNAGA), which possesses great biocompatibility and similarity to PNIPAM. The internal morphology, dynamic moduli, de-cross-linking properties, and temperature responsiveness of the hydrogels were systematically investigated. Upon hydrogen-bonding reinforcement, the hydrogel elasticity, reflected by the maximum storage modulus, dramatically increased from 90.2 to 517.0 kPa, which is about a 570% increase compared with unreinforced hydrogels. In addition, the mechanical properties of the hydrogel were reinforced as the de-cross-linking could be inhibited by PNAGA-based hydrogen-bonding. The temperature release behavior of the hydrogel was assessed with a model drug (propranolol hydrochloride, PHCl) and could be precisely controlled by adjusting the environmental temperature between 25 and 37 °C. Therefore, PNAGA reinforced thermoresponsive hydrogels are promising functional biological materials for use in tissue-repair engineering and controlled-release drug delivery.

研究领域: 生物材料 · 组织工程 · 药物递送系统
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TRIBOLOGY INTERNATIONAL · 2025 · IF 6.9

Hydrogen-bonding reinforced robust hydrogels for load-bearing and sustained lubrication

Ruiyao Ma,Yanru Liu,Huijuan Lin,Ling-Bao Xing,Hui Liu,Shuanhong Ma,Feng Zhou

The creation of bionic hydrogel characterized by optimal friction and load-bearing is essential for implantable artificial materials. High-stiffness and robust poly (methylacrylamide and methacrylic acid) hydrogels (P(MAAm-MAAc)) were synthesized using intensive cross-linking and intermolecular/intramolecular hydrogen bonding. Subsequently, an embedded lubricating layer was developed on the robust base, which formed layered structure similar to articular cartilage. It possesses distinctive mechanical characteristics (tensile strength: 3.9–4.4 MPa; elastic modulus: 27.8–38.6 MPa), along with superior lubricating and load-bearing capabilities. When water served as lubricant, the hydrogels exhibited low friction coefficient (COF ∼ 0.039), negligible wear, and sustained endurance over 18,000 sliding cycles. This high-stiffness and robust multilayer hydrogel possesses extensive application potential in bionic articular cartilage, medical devices, and other domains.

研究领域: 生物材料学 · 组织工程 · 生物摩擦学 · 再生医学 · 医用高分子材料
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POLYMER · 2017 · IF 3.684

Hydrogen bond reinforced poly(1-vinylimidazole-co-acrylic acid) hydrogels with high toughness, fast self-recovery, and dual pH-responsiveness

Hongyao Ding,Xin Ning Zhang,Si Yu Zheng,Yihu Song,Zi Liang Wu,Qiang Zheng

As a promising structural material, various tough hydrogels have been developed in recent years by incorporating different kinds of noncovalent bonds as the energy-dissipating segments. Among these systems, it is challenging to use hydrogen bonds due to their instability in aqueous environment. Here we report a tough hydrogel of poly(1-vinylimidazole- co -acrylic acid) (P(VI- co -AAc)) reinforced by the robust hydrogen bonds between imidazole and carboxylic acid groups. The hydrogels with different composition possess excellent mechanical performances, with tensile breaking stress, breaking strain, Young's modulus , and tearing fracture energy being 0.3–1.8 MPa, 920–1400%, 0.1–0.7 MPa, and 0.7–5.6 kJ/m 2 , respectively, which are well maintained over a wide pH range (3 ≤ pH ≤ 10). The high stability of hydrogen bonds should be rooted in the strong proton donor-acceptor pair. However, when pH ≤ 2 or pH ≥ 11, the gels become highly swelled due to the dissociation of imidazole and carboxylic acid groups, respectively, accompanying with dramatic decrease in mechanical properties . The tough hydrogels also show temperature- and deformation rate-dependent mechanical properties , as well as shape memory and self-recovery abilities, due to the dynamic nature of noncovalent bonds. Such hydrogels with remarkable mechanical properties and dual pH-responsiveness should find applications in load-bearing soft actuators, flexible electronics, etc.

CAS / MDL: 79-10-7 7727-21-1
研究领域: 材料科学 · 生物医学工程
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JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS · 2018 ·Vol. 56 ·期 19 ·1281-1286 · IF 2.499

Hydrogen bond-reinforced double-network hydrogels with ultrahigh elastic modulus and shape memory property

Yan Jie Wang,Chen Yu Li,Zhi Jian Wang,Yiping Zhao,Li Chen,Zi Liang Wu,Qiang Zheng

Development of tough hydrogels has greatly expanded their applications as load-bearing materials. However, the elastic modulus of tough hydrogels is usually lower than 1 MPa. It remains a challenge to design tough hydrogels with high modulus. We report here a series of tough double-network (DN) hydrogels with ultrahigh elastic modulus (up to 200 MPa) by forming robust hydrogen bonds between the first poly(acrylic acid) network and the second poly( N -isopropyl acrylamide) network. The dense cooperative hydrogen bonds greatly reduce the segmental mobility and thus improve the rigidity of gel matrix. Owing to the dynamic nature of hydrogen bonds, the modulus of hydrogels is strongly influenced by temperature and pH, affording the gels shape memory property. The strategy by forming robust noncovalent bonds between interpenetrating networks should be applicable to other systems for designing tough and versatile hydrogels with diverse promising applications. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56 , 1281–1286

研究领域: 高分子物理 · 生物材料 · 软物质科学 · 智能响应材料 · 组织工程
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Journal of Materials Chemistry A · 2025 · IF 9.5

Hydrogen-Bond Armored MXene Hydrogel for Oxidation-Resistant, Dual-Mode Wearable Sensors

Jiahao Liu,Jie Yang,Xueming Tang,Ruobing Tian,Guohua Zhang,Jiahang Yang,Yan Jiang,Yuanna Sun

Wearable MXene-based hydrogels hold significant promise for flexible electronics due to their tissue-compliant mechanics and exceptional electrical properties, yet their practical deployment is fundamentally challenged by MXene’s rapid oxidation in aqueous environments. To address this limitation, we develop an oxidation-resistant nanocomposite hydrogel through multi-hydrogen-bond reinforcement using poly (N-acryloyl glycinamide) (PNAGA), cellulose nanocrystals (CNC), and MXene. In this design, hydroxyl groups on CNC form robust hydrogen bonds simultaneously with the PNAGA network and MXene surface functional groups, establishing a ternary protective barrier that sterically isolates MXene from water/oxygen exposure while enhancing nanosheet dispersion and mechanical reinforcement. The resulting PNAGA-CNC-MXene (NCM) hydrogel achieves a high electrical conductivity of 0.59 S/m alongside superior mechanical properties. As an integrated sensor, it exhibits dual functionality: strain sensing with a gauge factor of 2.91 and 260 ms response speed, coupled with temperature detection at high sensitivity (-2.16 %/ºC) and 0.1 ºC resolution. Critically, Bluetooth-enabled wireless transmission facilitates real-time monitoring of physiological signals on mobile devices. This hydrogen-bond network strategy not only resolves MXene’s oxidation-stability conflict but also advances NCM hydrogels as versatile platforms for next-generation wearable electronics, personalized health monitoring, and human-machine interfaces.

CAS / MDL: 7727-21-1 7789-24-4
研究领域: 生物医学工程 · 柔性电子学 · 纳米复合材料 · 传感器技术 · 转化医学 · 人机接口
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