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Advanced Materials Interfaces · 2020 ·Vol. 7 ·期 15 ·2000485 · IF 4.948

Reducing Friction by Control of Isoelectric Point: A Potential Method to Design Artificial Cartilage

Shihua Yuan,Xinchun Chen,Chenhui Zhang

Relative motion between artificial cartilages is too slow to form a sufficient lubricating film for hydrodynamic lubrication, and this can result in large friction and wear. Hydration lubrication is effective in reducing friction at low speeds, and the lubricity is mostly determined by surface charges, which can be assessed by isoelectric point (IEP). Therefore, by controlling the IEP of friction pairs, ultralow friction can be achieved even with weak hydrodynamic lubrication. Here, a negatively charged material is synthesized by grafting carboxylate anions into an epoxy resin matrix. Compared with pristine epoxy resin (IEP = 6.0), the modified epoxy resins (IEP = 3.8, IEP = 3.0) show better tribological properties. In particular, at low speeds (4.7 and 1.2 mm s −1 ), the friction coefficients are as low as 0.02–0.04, and the average contact pressures are ≈10 MPa, when a NaCl solutions are used as the lubricants. Furthermore, the addition of hydroxyapatite to the modified epoxy resin not only increases its bioactivity, but also reduces friction. Superlubricity can be achieved for the speeds higher than 23.5 mm s −1 . These results provide a method to design artificial cartilage with good tribological and bearing capacity.

研究领域: 生物材料学 · 生物力学
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POLYMERS FOR ADVANCED TECHNOLOGIES · 2022 ·Vol. 33 ·期 10 ·3455-3469 · IF 3.348

Organic solvents enhance polyvinyl alcohol/polyethylene glycol self-healing hydrogels for artificial cartilage

Zishuo Ye,Hailin Lu,Endong Jia,Jian Chen,Lifeng Fu

Polyvinyl alcohol (PVA) hydrogels have potential applications in bionic articular cartilage due to their good biocompatibility and low friction. However, the lack of adequate mechanical properties is a key obstacle for PVA hydrogels to replace natural cartilage. In this study, polyethylene glycol (PEG) was introduced into the PVA hydrogel, and the (PVA/PEG) composite gels were prepared by a blending physical cross-linking method. The PVA/PEG gels were treated with a simple and novel organic solvent immersion dehydration to improve its mechanical and tribological properties. And the using of organic solvents for dehydration changed the network structure of the PVA/PEG gels, which improved the mechanical properties effectively. In this study, the effects of different organic solvents on the tribological properties, swelling ratio, shore hardness, and dehydration rate of PVA/PEG hydrogels were investigated. Compared with natural drying, organic solvent dehydration reduced the gel formation time. Notably, the organic solvent dehydration treatment reduces the wear rate of PE ball friction pair to 27.4% of the original amount, improving wear resistance. Meanwhile, self-healing and cellular immune assays demonstrated the excellent biocompatibility and self-healing ability of the PVA/PEG gels. This study provides a new candidate material for the design of articular cartilage, which is expected to advance the progress of artificial cartilage repair.

研究领域: 生物材料学 · 医学工程 · 组织工程
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Tough Engineering Hydrogels Based on Swelling–Freeze–Thaw Method for Artificial Cartilage

Mingming Hao,Yongfeng Wang,Lianhui Li,Yinhang Liu,Yuanyuan Bai,Weifan Zhou,Qifeng Lu,Fuqin Sun,Lili Li,Simin Feng,Wei Wei,Ting Zhang

Articular cartilage, which exhibits toughness and ultralow friction even under high squeezing pressures, plays an important role in the daily movement of joints. However, joint soft tissue lesions or injuries caused by diseases, trauma, or human functional decline are inevitable. Poly(vinyl alcohol) (PVA) hydrogels, which have a water content and compressive strength similar to those of many tissues and organs, have the potential to replace tough connective tissues, including cartilage. However, currently, PVA hydrogels are not suitable for complex dynamic environments and lack rebound resilience, especially under long-term or multicycle mechanical loads. Inspired by biological tissues that exhibit increased mechanical strength after swelling, we report a tough engineered hydrogel (TEHy) fabricated by swelling and freeze–thaw methods with a high compressive strength (31 MPa), high toughness (1.17 MJ m–3), a low friction coefficient (0.01), and a low energy loss factor (0.22). Notably, the TEHy remained remarkably resilient after 100 000 cycles of contact extrusion and remains intact after being compressed by an automobile with a weight of approximately 1600 kg. The TEHy also exhibited excellent water swelling resistance (volume and weight changes less than 5%). Moreover, skeletal muscle cells were able to readily attach and proliferate on the surface of TEHy-6, suggesting its outstanding biocompatibility. Overall, this swelling and freeze–thaw strategy solves the antifatigue and stability problems of PVA hydrogels under large static loads (>10 000 N) and provides an avenue to fabricate engineering hydrogels with strong antifatigue and antiswelling properties and ultralow friction for potential use as biomaterials in tissue engineering.

CAS / MDL: 9004-61-9 9002-89-5
研究领域: 生物医学工程 · 材料科学 · 组织工程
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Journal of Materials Chemistry B · 2019 ·Vol. 8 ·期 4 ·677-690 · IF 5.047

3D printing of a poly(vinyl alcohol)-based nano-composite hydrogel as an artificial cartilage replacement and the improvement mechanism of printing accuracy

Yeqiao Meng,Jinlong Cao,Yue Chen,Yaru Yu,Lin Ye

Inspired by the gradient structure of articular cartilage, a poly(vinyl alcohol) (PVA)-based composite hydrogel with a biomimetic gradient structure as an artificial cartilage replacement was constructed by an extrusion 3D printing technique. The influence of the concentration and composition of the PVA-based solution on its rheological behavior and printability was studied, and the improvement mechanism for the 3D printing accuracy of the hydrogel was explored: introduction of GO or GO–HA gave rise to weakened inter-molecular hydrogen bonds and reduced entanglement density simultaneously, and the dynamic viscosity was highly improved. Therefore, the solution exhibited enhanced shear-thinning behavior in the printing shear rate range and a reduced Barus effect, thus highly improving the printability and printing accuracy of the samples. The 3D printing of PVA hydrogels was successfully achieved, and the printed biomimetic gradient samples possessed suitable compressive and tribological properties, which showed promising potential in the precise customized repair of artificial cartilage.

研究领域: 生物材料学 · 医学工程 · 组织工程
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BIOMACROMOLECULES · 2025 · IF 5.4

Enhanced Lubrication through Porous Hydrogels Anchored with Hyaluronic Acid

Yanli Gong,Ying Xiang,Qi Li,Yingxin Li,Wenlang Liang,Sha Li,Yong-Xiang Leng

Achieving sustained low-friction in hydrogels is often hindered by poor retention of boundary lubricants like hyaluronic acid (HA). Here, we report a multiphase hydrogel designed to actively manage HA lubrication. We fabricated a porous poly(vinyl alcohol) (PVA) hydrogel matrix containing polycationic chitosan quaternary ammonium salts (PQCS). This interconnected porous architecture serves a dual role: it acts as a reservoir for HA, while the PQCS provides electrostatic anchoring sites to control HA retention and release. Under load, this structure facilitates the extrusion of anchored HA to the sliding interface, establishing a continuous and self-replenishing boundary lubrication layer. Consequently, the hydrogel anchored with high-molecular-weight HA achieved a sustained and low coefficient of friction (COF < 0.05) in PBS solution. This strategy of engineering internal architecture to control lubricant dynamics at the interface offers a promising approach for designing advanced self-lubricating biomaterials like artificial cartilage.

CAS / MDL: 9002-89-5
研究领域: 生物材料学 · 组织工程 · 摩擦学 · 高分子科学 · 再生医学
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POLYMER INTERNATIONAL · 2022 ·Vol. 72 ·期 1 ·27-38 · IF 3.213

Glycerol-modified poly(vinyl alcohol)/poly(ethylene glycol) self-healing hydrogel for artificial cartilage

Zishuo Ye,Hailin Lu,Guiquan Chai,Changlei Wu,Jian Chen,Leifeng Lv

Poly(vinyl alcohol) (PVA) hydrogels have shown potential applications in bionic articular cartilage due to their tissue-like viscoelasticity, good biocompatibility and low friction. However, their lack of adequate mechanical properties is a key obstacle for PVA hydrogels to replace natural cartilage. In this study, poly(ethylene glycol) (PEG) and glycerol were introduced into PVA, and a PVA/PEG–glycerol composite hydrogel was synthesized using a mixing physical crosslinking method. The mechanical properties, hydrophilicity and tribological behavior of the PVA/PEG–glycerol hydrogel were investigated by changing the concentration of glycerol in PEG. The results showed that the tensile strength of the hydrogel reached 26.6 MPa at 270% elongation at break with 20 wt% of glycerol plasticizer, which satisfied the demand of natural cartilage. In addition, the excellent hydrophilicity of glycerol provides good lubricating properties for the composite gel under dry friction. Meanwhile, self-healing and cellular immunity assays demonstrated that the composite gel could have good self-healing ability and excellent biocompatibility even in the absence of external stimuli. This study provides a new candidate material for the design of articular cartilage, which has the potential to facilitate advances in artificial joint cartilage repair. © 2022 Society of Industrial Chemistry.

CAS / MDL: 9002-88-4
研究领域: 材料科学 · 生物医学工程 · 组织工程
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Coatings · 2025 ·Vol. 15 ·期 8 ·893 · IF 2.8

High-Performance Sodium Alginate Fiber-Reinforced Polyvinyl Alcohol Hydrogel for Artificial Cartilage

Lingling Cui,Yifan Lu,Jun Wang,Haiqin Ding,Guodong Jia,Zhiwei Li,Guang Ji,Dangsheng Xiong

Hydrogels, especially Polyvinyl alcohols, have received extensive attention as alternative materials for articular cartilage. Aiming at the problems such as low strength and poor toughness of polyvinyl alcohol hydrogels in practical applications, an enhancement and modification strategy is proposed. Sodium alginate fibers were introduced into polyvinyl alcohol hydrogel network through physical blending and freezing/thawing methods. The prepared composite hydrogels exhibited a three-dimensional porous network structure similar to that of human articular cartilage. The mechanical and tribological properties of hydrogels have been significantly improved, due to the multiple hydrogen bonding interaction between sodium alginate fibers and polyvinyl alcohol. Most importantly, under a load of 2 N, the friction coefficient of the PVA/0.4SA hydrogel can remain stable at 0.02 when lubricated in PBS buffer for 1 h. This work provides a novel design strategy for the development of high-performance polyvinyl alcohol hydrogels.

CAS / MDL: 9002-89-5 9005-38-3
研究领域: 生物医学材料 · 高分子科学 · 组织工程 · 材料科学 · 机械工程
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A novel protocol for injectable artificial cartilage constructs based on programmed shape-morphing hydrogels for cartilage regeneration

Qi Lv,Chunhui Ma

Direct contact between cells is of great significance to the formation of natural tissues, especially in regard to cartilage differentiation, which begins with the biological process of cell aggregation. Herein, based on the preparation of microspheres via microwells, we prepared functional hydrogel-based microwells by using cobalt ionic crosslinking. The preparation of functional microwells can not only induce the upregulation of genes and proteins related to cartilage differentiation but also greatly reduce markers related to hypertrophy and mineralization, which play a significant role in the formation of hyaline cartilage. Importantly, we combined microwell cultures with the later preparation of injectable artificial cartilage grafts. In vitro, microwell culture and cartilage differentiation induction can be achieved through the preparation of microwells crosslinked by ions. Via the partial removal of ions, the hydrogel and microtissues can be injected into the defect through the shape recovery of the gel in the later stage and through the stable gel formed by covalent crosslinking to repair irregular cartilage defects. This study not only broadens the application of microwells but also promotes the progress of material-based tissue engineering strategies through the design of intelligent materials.

研究领域: 生物医学工程 · 组织工程 · 材料科学
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Materials Today Physics · 2024 · IF 10

Tough double-network hydrogels with excellent frictional properties based on the in-suit inhibition strategy for biomedical applications

Junyu Wang,Xiaomin Li,Yan Xu,Shenglin Li,Jian Song,Yuhong Liu

Osteoarthritis (OA) is one of the most common joint disorders all over the world and hydrogels could be an effective tool to solve this problem. In this work, we explore the mechanism of tribology properties of double-network hydrogel (DN hydrogel) under effect of free radical polymerization inhibitors. Fe 3+ is added to the DN hydrogel as highly efficient and easily adjustable inhibitor, and the friction coefficient can be reduced to 0.0038 by adjusting the concentration. Even after 6 h of continuous tribological testing, the DN hydrogel remains a surprising sustained superlubricity. Furthermore, the strength of the hydrogel can reach 2.36 MPa, which is 20 times higher than that of the single-network hydrogel (SN hydrogel). The introduction of the inhibitor reduces covalent crosslinking that enables the hydrogel to form a sparser mesh structure conducive to the reduction of the friction coefficient, especially the additional physical cross-linking delivered from the electrostatic interaction between Fe 3+ and carboxyl groups increases strength. The optimum concentration of Fe 3+ is explored to achieve the synergetic improvement of lubricative and mechanical properties. This work opens innovative technology routes for developing superlubricious and tough hydrogels, which is a brighter future for artificial cartilage applications.

CAS / MDL: 79-10-7
研究领域: 材料科学 · 生物医学工程 · 摩擦学
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POLYMER · 2019 · IF 3.771

Mechanically robust, notch-insensitive, fatigue resistant and self-recoverable hydrogels with homogeneous and viscoelastic network constructed by a novel multifunctional cross-linker

Yi Wang,Jinrong Wu,Zhenxing Cao,Changshu Ma,Qingbo Tong,Jiangbo Li,Hanchao Liu,Jing Zheng,Guangsu Huang

Designing a homogeneous network is an efficient way to improve the mechanical properties of hydrogels. However, the homogeneous hydrogels usually have negligible notch-insensitivity due to the lack of effective energy dissipation, limiting their practical applications in many fields. Herein, we provide a straightforward method to prepare a category of tough and notch-insensitive polyacrylamide hydrogels crosslinked by a novel cross-linker with multiple vinyl functional groups (TA). Due to the multifunctionality of TA , a relatively uniform network with the coexistence of physical cross-links is constructed by the steric effect between chain radicals on TA molecules during the polymerization. The uniform network distributes stress evenly while the physical cross-links lead to viscoelastic dissipated energy under external force. As a result, the hydrogels achieve an ultrastretchability of 2400% and a tensile toughness of 4.33 MJ/m 3 . Even with a notch of 10 mm, the hydrogels can still be stretched to a strain of 20, indicating an impressive notch-insensitivity. Meanwhile, the hydrogels exhibit high fatigue resistance and good self-recovery. This research offers a facile strategy for designing high-performance hydrogels and may pave the way for their practical application in emerging fields, such as oil displacement agent and artificial cartilage .

CAS / MDL: 57-13-6
研究领域: 材料科学 · 聚合物化学 · 生物医学工程
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