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CHEMISTRY OF MATERIALS · 2025 · IF 7

Bioinspired Structure with Hierarchical Hydrogen Bonding and Metal Coordination for Enhanced Properties of Biobased Polyurethane Applied in Artificial Ligaments

Junjie Wang,Xiaoyu Dong,Haojie Qiu,Zhixiu Liu,Yufeng Kang,Jinghua Du,Xuefeng Yang,Xue-liang Li,Yunsheng Ding

The utilization of biobased polyurethanes in medical engineering is constrained by their inferior mechanical properties. A variety of strategies that aim to improve the mechanical properties of these materials have been developed to meet the specific requirements of biomedical applications. Inspired by the chemical structure of the jawbone of a marine worm called Nereis, the polymer chain can be coordinated with zinc ions to improve biobased polyurethane mechanical properties. In this study, a series of biobased polyurethanes were synthesized via a prepolymerization process involving the usage of biobased polycarbonate diol in conjunction with lysine diisocyanate and isophorone diisocyanate, followed by the addition of isophorone diamine and 2-amino-5-(2-hydroxyethyl)-6-methylpyrimidin-4-ol to complete the chain expansion along with the addition of Zn2+ for coordination. The mechanical properties (including tensile, cycling, and fatigue resistance) and biocompatibility of the biobased polyurethanes were evaluated through a series of tests. The resulting biobased polyurethane, comprising a bioinspired syngeneic structure, exhibited remarkable properties, including a tensile strength of 40.6 MPa, a toughness of 147.6 MPa/m3, and an energy recovery of 91.6%, which represents a 167% improvement in toughness compared to the biobased polyurethane without metal coordination. Furthermore, the biobased polyurethane with the syngenetic effect of hierarchical hydrogen bonding and metal coordination retains 80.2% of its strength after 300 cycles without any crack propagation. In addition, the good biocompatibility of biobased polyurethanes indicates the possibility of in vivo bioapplication, so they should have potential application in artificial ligaments.

研究领域: 材料科学 · 生物医学工程 · 组织工程
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COMPOSITES PART B-ENGINEERING · 2024 · IF 12.7

Directional anneal-casting strategy enables mechanically enhanced biomimetic hydrogel for ligament reconstruction

He Zhu,Cheng Wang,Chen Xin,Ziyi Dai,Yican Yang,Yan Li,Mingrui Wang,Yang Zhang,Shouwei Yue,Rong Cai,Kai Qian

Artificial ligaments play a crucial role in replacing injured natural ligaments and facilitating rehabilitation. However, existing artificial ligaments lack real-time strain monitoring capability, which limits personalized rehabilitation guidance. Here, we develop a highly biomimetic and intelligent electronic hydrogel ligament (IEHL) based on polyvinyl alcohol/sodium alginate through a universal directional anneal-casting (DAC) strategy. This innovative approach creates aligned microstructures that overcome conventional hydrogels' limitations of poor structural integrity and inadequate mechanical properties. The IEHL exhibits integrated bionics of microstructure, mechanical parameters and water content closely matching natural ligaments. The efficacy of the IEHL in stabilizing knee joint and monitoring movements is validated through in vivo models, and a wireless monitoring system is developed to detect and analyze ligament strain characteristics in real-time. This IEHL provides a superior intraoperative replacement strategy and quantitative guidance for post-surgical rehabilitation.

CAS / MDL: 9002-89-5
研究领域: 生物材料学 · 再生医学 · 运动医学
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APPLIED SURFACE SCIENCE · 2011 · IF 1.795

Composite coating of 58S bioglass and hydroxyapatite on a poly (ethylene terepthalate) artificial ligament graft for the graft osseointegration in a bone tunnel

Hong Li,Yang Wu,Yunsheng Ge,Jia Jiang,Kai Gao,Pengyun Zhang,Lingxiang Wu,Shiyi Chen

The purpose of this study was to determine the effect of the combination of hydroxyapatite (HA) and bioglass (BG) on polyethylene terephthalate (PET) artificial ligament graft osseointegration within the bone tunnel. The results of in vitro culturing of MC3T3-E1 mouse osteoblastic cells proved that this HA/BG composite coating can promote the cell compatibility of grafts. A rabbit extraarticular tendon-to-bone healing model was used to evaluate the effect of this composite coating on PET artificial ligaments in vivo. The final results demonstrated that HA/BG coating improved new bone formation at the graft-bone interface and increased the load-to-failure property of graft in bone tunnel compared to the control group at early time. The study has shown that HA/BG composite coating on the PET artificial ligament surface has a positive effect in the induction of artificial ligament osseointegration within the bone tunnel.

研究领域: 生物材料学 · 骨科医学
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INTERNATIONAL ORTHOPAEDICS · 2010 ·Vol. 35 ·期 10 ·1561-1567 · IF 1.825

Hydroxyapatite coating enhances polyethylene terephthalate artificial ligament graft osseointegration in the bone tunnel

Li Hong,Ge Yunsheng,Wu Yang,Jiang Jia,Gao Kai,Zhang Pengyun,Wu Lingxiang,Chen Shiyi

The purpose of this study was to investigate whether hydroxyapatite (HAp) coating could induce polyethylene terephthalate (PET) artificial ligament graft osseointegration in the bone tunnel. Twenty-four New Zealand white rabbits underwent artificial ligament graft transplantation in bilateral proximal tibia tunnels. One limb was implanted with HAp-coated PET graft, and the contralateral limb was implanted with non-HAp-coated PET graft as control. The rabbits were randomly sacrificed at four and eight weeks after surgery. The loads to failure of the experimental group at eight weeks were significantly higher than those of the control group ( p  = 0.0057). Histologically, application of HAp coating induced new bone formation between graft and bone at eight weeks compared with the controls. Real-time polymerase chain reaction examination revealed significantly elevated messenger ribonucleic acid expression levels of osteopontin and collagen I in the grafts of the HAp group compared with the controls at four weeks ( p  < 0.05). The study has shown that HAp coating on the PET artificial ligament surface has a positive effect in the induction of artificial ligament osseointegration within the bone tunnel.

研究领域: 骨科 · 生物材料 · 组织工程
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Frontiers in Bioengineering and Biotechnology · 2021 · IF 5.89

Preparation and Properties of Antibacterial Polydopamine and Nano-Hydroxyapatite Modified Polyethylene Terephthalate Artificial Ligament

Wu Yang,Zhang Yuhan,Zhang Ren,Chen Shiyi

Due to its great biomechanical property, the polyethylene terephthalate (PET) artificial ligament has become one of the most promising allografts for anterior cruciate ligament (ACL) reconstruction. However, because of its chemical and biological inertness, PET is not a favored scaffold material for osteoblast growth, which promotes the ligament-bone healing. Meanwhile, in consideration of prevention of potential infection, the prophylactic injection of antibiotic was used as a post-operative standard procedure but also has the increasing risk of bacterial resistance. To face these two contradictions, in this article we coated a polydopamine (PDA) nano-layer on the PET ligament and used the coating as the adhesion interlayer to introduce nano-hydroxyapatite (nHA) and silver atoms to the surface of PET ligament. Because of the mild self-polymerization reaction of dopamine, the thermogravity analysis (TGA), Raman spectrum, and tensile test results show that the modification procedure have no negative effects on the chemical stability and mechanical properties of the PET. The results of NIH3T3 cell culture show that the PDA and nHA could effectively improve the biocompatibility of PET artificial ligament for fibroblast growth, and staphylococcus aureus antibacterial test results show that the Ag atom provided an antibacterial effect for PET ligament. As shown in this paper, the nano-PDA coating modification procedure could not only preserve the advantages of PET but also introduce new performance characteristics to PET, which opens the door for further functionalization of PET artificial ligament for its advanced development and application.

CAS / MDL: 1306-06-5 12167-74-7
研究领域: 生物材料学 · 骨科医学 · 组织工程学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

A Mechanoluminescence-Based Stress Sensing Hydrogel for Intelligent Artificial Ligament

Chunmei Yan,Xiao He,Bo Yu,Bo Zhou,Shaofan Fang,Jia Xu,Bin Liu,Zhaofeng Wang

Robust and biocompatible hydrogels are recognized as promising biomimetic soft materials to improve human life quality. To ensure their stable, reliable, and safe service, the hydrogels are further required to have non-contact and wireless stress sensing ability. Herein, a mechanoluminescence (ML) based micellar hydrogel is developed, in which the surface-modified BaSi 2 O 2 N 2 : Eu 2+ (M-BSON) particles are chemically incorporated into the cross-linked polyacrylamide/polymethyl acrylate (PAM/PMA) network structure. Because of the interactions between the M-BSON particles and the PMA micelles, the as-fabricated composite hydrogel exhibits enhanced mechanical properties with a mechanical strength of 2.73 MPa and a toughness of 3.40 MJ m −3 , respectively. The chemical wrapping of the M-BSON particles by the hydrophobic PMA micelles further protects the ML properties from water quenching, leading to remarkable stress-induced luminescence under the water environment of hydrogel. Because of its desirable mechanical performance, attractive stress-light responsiveness, and good biocompatibility, the M-BSON incorporated hydrogel has the potential to be applied as an intelligent artificial ligament for stress self-monitoring and failure warning. This work addresses the inhomogeneous dispersion and water quenching issues of the ML particles in hydrogel structure, which significantly promote ML applications in bionic engineering.

研究领域: 材料科学 · 生物医学工程 · 机械工程
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Small · 2024 · IF 13

Stepwisely Assembled Multicomponent Fiber with High Water Content and Superior Mechanical Properties for Artificial Ligament

Hao Huang,Weijie Wang,Zexin Liu,Hanxin Jian,Bing Xue,Liping Zhu,Kan Yue,Shuguang Yang

The ligament, which connects bones at the joints, has both high water content and excellent mechanical properties in living organisms. However, it is still challenging to fabricate fibrous materials that possess high water content and ligament-like mechanical characteristics simultaneously. Herein, the design and preparation of a ligament-mimicking multicomponent fiber is reported through stepwise assembly of polysaccharide, calcium, and dopamine. In simulated body fluid, the resulting fiber has a water content of 40 wt%, while demonstrating strength of ≈120 MPa, a Young's modulus of ≈3 GPa, and a toughness of ≈25 MJ m −3 . Additionally, the multicomponent fiber exhibits excellent creep and fatigue resistance, as well as biocompatibility to support cell growth in vitro. These findings suggest that the fiber has potential for engineering high-performance artificial ligament.

研究领域: 生物材料 · 组织工程 · 机械工程 · 生物医学工程
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