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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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Biomaterials Science · 2016 ·Vol. 4 ·期 11 ·1673-1681 · IF 3.614

A thermoresponsive supramolecular copolymer hydrogel for the embolization of kidney arteries

Xiaohuan Shi,Haijun Gao,Fengying Dai,Xuequan Feng,Wenguang Liu

Our team has previously reported a high strength thermoplastic supramolecular polymer hydrogel. However, the hydrogel required injection temperatures outside the physiological range therefore preventing its use in a living environment. In this article, we reported a thermoresponsive supramolecular copolymer hydrogel p(N-acryloyl glycinamide-co-acrylamide) (PNAGA-PAAm), which can be injected at temperatures within the physiological range. We used rheological measurements to demonstrate that the transition temperature (upper critical solution temperature) of both the moduli and gel–sol could be finely adjusted by controlling both the ratio and concentration of the monomer. Adding iohexol (contrast agent) in PNAGA-PAAm hydrogels contributed to the decreased moduli and gel–sol transition temperature due to weakening of the hydrogen bonding interactions. The cytocompatible and hemocompatible PNAGA-PAAm sol mixed with iohexol was injected into the renal arteries of rabbits through a microcatheter at a temperature within the high biological range. The transition from the injection temperature (high biological range) to body temperature (basal for the animals) quickly solidified the embolic agent without the occurrence of dehydration, therefore overcoming the main limitation of LCST-typed poly(N-isopropylacrylamide) previously reported. Angiography and histological examination demonstrated the successful embolization of both renal arteries and no recanalization was observed after 8 weeks. The PNAGA-based supramolecular copolymer hydrogel is a novel embolic agent that allows for the occlusion of larger sized arteries in a biocompatible environment.

研究领域: 生物医学工程 · 材料科学 · 医学
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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2021 ·Vol. 222 ·期 6 ·2000429 · IF 2.527

A Facile Strategy to Achieve Synergistic Multiple Hydrogen Bonding Interactions for Constructing Robust Hydrogels with Self-healing Capability, Shape Transformation and Actuation Function

Jumin Yang,Valenzuela Cristian,Anjie Dong,Jianhua Zhang

The double network (DN) hydrogels, especially the physically crosslinked DN hydrogels, have attracted increasing attention due to their high reconfigurability, multi-sensitivity, and efficient energy dissipation, but their applications still suffer from the relatively low mechanical strength, complex preparation process, and insufficient functionality. In this work, a simple but efficient strategy to fabricate robust and multitasking polyvinyl alcohol (PVA)/poly( N -acryloyl glycinamide) (PNAGA) DN hydrogels via an ultraviolet (UV)-initiated one-pot in situ polymerization and a subsequent freezing-thawing treatment is reported. The PVA/PNAGA DN hydrogels are fully physically linked DN network via multiple hydrogen bonding interactions, which contain hard PVA crystalline microdomains and soft PNAGA regions. The synergetic multiple hydrogen bonding interactions and the cooperation of hard and soft regions in PVA/PNAGA hydrogels as well as the polyhydroxy matrix can not only impart the PVA/PNAGA hydrogels with super mechanical strength, high toughness, good stretchability, and rapid shape-recoverability, but also endow the hydrogels with tailorable self-healability, multiple shape memory, and actuation function. Considering the easily available materials, simple preparation process, and highly multitasking properties, this novel strategy should greatly enrich the methodological toolbox for the synthesis of robust and multifunctional hydrogels for the diversity of applications.

CAS / MDL: 1303-96-4
研究领域: 材料科学 · 高分子化学 · 软物质物理
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Journal of Materials Chemistry B · 2020 ·Vol. 9 ·期 1 ·176-186 · IF 5.344

Tough thermoplastic hydrogels with re-processability and recyclability for strain sensors

Xiaohua Zhang,Xuefeng Yang,Qiyuan Dai,Yichen Zhang,Haotian Pan,Chenxi Yu,Qi Feng,Shuangli Zhu,Hua Dong,Xiaodong Cao

Tough hydrogels with the ability to be repeatedly processed into various shapes as thermoplastics are highly desired in advanced medical devices and tissue engineering. Here, we have developed a kind of versatile supramolecular hydrogel with a network cross-linked by double hydrogen bonds from poly(N-acryloyl glycinamide) (PNAGA). The resulting PNAGA-30 hydrogels (30 wt% solid content) are tough, re-processable, and recyclable similar to thermoplastics. The hydrogels in the form of fragments can be easily re-processed into various shapes including sheet, filament, cylinder and other complex shapes by using simple stamping and injection methods. The mechanical properties of the re-programed hydrogels are comparable to the properties of the original hydrogels. The re-processability and robust mechanical properties of the PNAGA hydrogels are promising for practical applications in soft materials, tissue engineering and wearable devices. Furthermore, the PNAGA-30&LiCl ionic hydrogels can be fabricated by simply compositing LiCl into thermoplastic hydrogels. The PNAGA-30&LiCl hydrogels can function as multifunctional strain sensors to monitor large human movements and tiny vibrations, thereby showing great application potential in robotics, biomedical prosthetics, personal healthcare monitoring and so on.

研究领域: 材料科学 · 生物医学工程 · 组织工程 · 可穿戴技术 · 机器人技术 · 健康监测
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