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Chitosan-based thermosensitive hydrogel with long-term release of murine nerve growth factor for neurotrophic keratopathy

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Neural Regeneration Research 2024年第3期19卷 680-686页

作者： Jie Wu Yulei Huang Hanrui Yu Kaixiu Li Shifeng Zhang Guoqing Qiao Xiao Liu Hongmei Duan Yifei Huang Kwok-Fai So Zhaoyang Yang Xiaoguang Li Liqiang Wang Department of Ophthalmology the Third Medical CenterChinese PLA General HospitalBeijingChina The PLA Medical College Department of NephrologyChinese PLA Institute of NephrologyState Key Laboratory of Kidney DiseasesNational Clinical Research Center for Kidney DiseasesBeijingChina Department of Ophthalmology Hainan Hospital of Chinese PLA General HospitalSanyaHainan ProvinceChina Medical School of Chinese PLA BeijingChina Department of Neurobiology School of Basic Medical SciencesCapital Medical UniversityBeijingChina Guangdong-Hongkong-Macao Institute of CNS Regeneration Ministry of Education CNS Regeneration Collaborative Joint LaboratoryJinan UniversityGuangzhouGuangdong ProvinceChina Bioland Laboratory(Guangzhou Regenerative Medicine and Health Guangdong Laboratory) GuangzhouGuangdong ProvinceChina Department of Ophthalmology and State Key Laboratory of Brain and Cognitive Sciences The University of Hong KongHong Kong Special Administrative RegionChina Center for Brain Science and Brain-Inspired Intelligence Guangdong-Hong Kong-Macao Greater Bay AreaGuangzhouGuangdong ProvinceChina Co-innovation Center of Neuroregeneration Nantong UniversityNantongJiangsu ProvinceChina School of Engineering Medicine Beijing Key Laboratory for Biomaterials and Neural RegenerationBeihang UniversityBeijingChina Beijing International Cooperation Bases for Science and Technology on Biomaterials and Neural Regeneration Beijing Advanced Innovation Center for Big Data-Based Precision MedicineBeihang UniversityBeijingChina

Neurotrophic keratopathy is a persistent defect of the corneal epithelium,with or without stromal ulceration,due to corneal nerve deficiency caused by a variety of etiologies.The treatment options for neurotrophic keratopathy are limited.In this study,an ophthalmic solution was constructed from a chitosan-based thermosensitive hydrogel with long-term release of murine nerve growth factor(CTH-mNGF).Its effectiveness was evaluated in corneal denervation(CD)mice and patients with neurotrophic keratopathy.In the preclinical setting,CTH-mNGF was assessed in a murine corneal denervation model.CTH-mNGF was transparent,thermosensitive,and ensured sustained release of mNGF for over 20 hours on the ocular surface,maintaining the local mNGF concentration around 1300 pg/mL in vivo.Corneal denervation mice treated with CTH-mNGF for 10 days showed a significant increase in corneal nerve area and total corneal nerve length compared with non-treated and CTH treated mice.A subsequent clinical trial of CTH-mNGF was conducted in patients with stage 2 or 3 neurotrophic keratopathy.Patients received topical CTH-mNGF twice daily for 8 weeks.Fluorescein sodium images,Schirmer’s test,intraocular pressure,Cochet-Bonnet corneal perception test,and best corrected visual acuity were evaluated.In total,six patients(total of seven eyes)diagnosed with neurotrophic keratopathy were enrolled.After 8 weeks of CTH-mNGF treatment,all participants showed a decreased area of corneal epithelial defect,as stained by fluorescence.Overall,six out of seven eyes had fluorescence staining scoresthermosensitive,and has sustained-release properties.Its effectiveness in healing corneal epithelial defects in

关键词： chitosan corneal reinnervation murine nerve growth factor neurotrophic keratopathy thermosensitive hydrogel

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Bioinspired metal-organic framework nanozyme reinforced with thermosensitive hydrogel for regulating inflammatory responses in Parkinson’s disease

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Nano Research 2024年第2期17卷 858-865页

作者： Xiaowan Fan Tao Zhang Xin Ding Yushuo Gu Qing Li Wei Jiang Kelong Fan Nanozyme Medical Center Academy of Medical ScienceZhengzhou UniversityZhengzhou 450001China Department Central-China Branch of National Center for Cardiovascular DiseasesHean Cardiovascular Disease CenterFuwai Central-China HospitalCentral China Fuwai Hospital of Zhengzhou UniversityZhengzhou 450046China Application Center for Precision Medicine the Second Affiliated Hospital of Zhengzhou UniversityZhengzhou 450052China CAS Engineering Laboratory for Nanozyme Key Laboratory of Protein and Peptide PharmaceuticalsInstitute of BiophysicsChinese Academy of SciencesBeijing 100101China University of Chinese Academy of Sciences Beijing 101408China Department of General Surgery Strategic Support Force Medical CenterBeijing 100101China Department of Anesthesiology Pain and Perioperative MedicineThe First Affiliated Hospital of Zhengzhou UniversityZhengzhou 450052China

Parkinson’s disease(PD)is a prevalent neurodegenerative disorder accompanied by movement disorders and neuroinflammatory injury.Anti-inflammatory intervention to regulate oxidative stress in the brain is beneficial for managing PD.However,traditional natural antioxidants have failed to meet the clinical treatment demands due to insufficient activity and sustainability.Herein,Cu-doping zeolite imidazolate framework-8(ZIF-8)nanozyme is designed to simulate Cu/Zn superoxide dismutase(SOD)by biomimetic mineralization.The nanozyme composite is then integrated into thermosensitive hydrogel(poly(lactic-co-glycolic acid)-poly(ethylene glycol)-poly(lactic-co-glycolic acid)(PLGA-PEG-PLGA))to form an effective antioxidant system(Cu-ZIF@hydrogel).The thermosensitive hydrogel incorporating nanozymes demonstrate distinct viscoelastic properties aimed at enhancing local nanozyme adhesion,prolonging nanozyme retention time,and modulating antioxidant activity,thus significantly improving the bioavailability of nanozymes.At the cellular and animal levels of PD,we find that Cu-ZIF@hydrogel bypass the blood-brain barrier and efficiently accumulate in the nerve cells.Moreover,the Cu-ZIF@hydrogel significantly alleviate the PD’s behavioral and pathological symptoms by reducing the neuroinflammatory levels in the lesion site.Therefore,the hydrogel-incorporating nanozyme system holds great potential as a simple and reliable avenue for managing PD.

关键词： bioinspired nanozyme thermosensitive hydrogel Parkinson’s disease oxidative stress neuroinflammatory

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Synergistic injection of the thermosensitive hydrogel and Bi-based alloy bone cement for orthopaedic repair

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Science China Technological Sciences 2024年第7期67卷 2153-2163页

作者： LIU SiCong LI Lei JIANG ChanYuan WANG QianYu DENG ZhongShan Key Laboratory of Cryogenic Science and Technology Technical Institute of Physics and Chemistry Chinese Academy of Sciences School of Future Technology University of Chinese Academy of Sciences Department of Cleft Lip and Palate Plastic Surgery Hospital Chinese Academy of Medical Sciences and Peking Union Medical College

Low-melting-point alloys have the advantages of good biocompatibility, plasticity, and near-bone mechanical strength, making them suitable as bone defect-filling materials for direct injection into defective bone sites. However, using low-melting-point alloys for orthopedic implants poses the challenge of causing thermal damage to the surrounding bone tissue during injection. In this study, a thermosensitive hydrogel is prepared and synergistically injected into the bone defect site with BiInSn. BiInSn solidifies and releases heat during injection, while the thermosensitive hydrogel absorbs heat and transforms into a gel state,encapsulating BiInSn. Therefore, the surrounding bone tissue is effectively protected from thermal damage. When BiInSn and the thermosensitive hydrogel were injected synergistically, in vitro thermal experiments revealed that the maximum temperature of the surrounding bone tissue reached 42°C. This temperature is below the 47°C threshold, which causes permanent damage to bone tissues. In vivo experiments demonstrated that rats in the BiInSn-thermosensitive hydrogel group exhibited better recovery at the bone defect sites. These results suggest that the synergistic injection of Bi-based alloy and thermosensitive hydrogel is beneficial in reducing thermal damage to bone tissue, guiding bone tissue growth, and effectively facilitating the repair of bone defects.

关键词： bone defects thermosensitive hydrogel thermal damage to tissue bismuth-based alloy bone cement

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A novel sprayable thermosensitive hydrogel coupled with zinc modified metformin promotes the healing of skin wound

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Bioactive Materials 2023年第2期20卷 610-626页

作者： Zhengwei Liu Wanze Tang Jiayi Liu Yingying Han Qinnan Yan Yuechao Dong Xiaomei Liu Dazhi Yang Guixing Ma Huiling Cao Department of Biochemistry School of MedicineSouthern University of Science and TechnologyGuangdong Provincial Key Laboratory of Cell Microenvironment and Disease ResearchShenzhen Key Laboratory of Cell MicroenvironmentShenzhen518055China Southern University of Science and Technology Shenzhen518055China Department of Biomedical Engineering Southern University of Science and TechnologyShenzhen518055China The First Affiliated Hospital Southern University of Science and TechnologyShenzhen518055China

A novel sprayable adhesive is established(ZnMet-PF127)by the combination of a thermosensitive hydrogel(Pluronic F127,PF127)and a coordination complex of zinc and metformin(ZnMet).Here we demonstrate that ZnMet-PF127 potently promotes the healing of traumatic skin defect and burn skin injury by promoting cell proliferation,angiogenesis,collagen formation.Furthermore,we find that ZnMet could inhibit reactive oxygen species(ROS)production through activation of autophagy,thereby protecting cell from oxidative stress induced damage and promoting healing of skin wound.ZnMet complex exerts better effects on promoting skin wound healing than ZnCl2 or metformin alone.ZnMet complex also displays excellent antibacterial activity against Staphylococcus aureus or Escherichia coli,which could reduce the incidence of skin wound infections.Collectively,we demonstrate that sprayable PF127 could be used as a new drug delivery system for treatment of skin injury.The advantages of this sprayable system are obvious:(1)It is convenient to use;(2)The hydrogel can cover irregular skin defect sites evenly in a liquid state.In combination with this system,we establish a novel sprayable adhesive(ZnMet-PF127)and demonstrate that it is a potential clinical treatment for traumatic skin defect and burn skin injury.

关键词： thermosensitive hydrogel Skin wound ZnMet-PF127 Reactive oxygen species(ROS) Autophagy

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Quaternized chitosan/Pluronic F127 thermosensitive hydrogel with high antibacterial properties for wound dressing

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Progress in Natural Science:Materials International 2023年第5期33卷 581-592页

作者： Kaiting Cheng Yiming Fang Liang Bai Feng Gui Junchi Ma Huimin Gao Yadong Zhao Xingtao Xu Marine Science and Technology College Zhejiang Ocean University Anhui Snow Dragon Fibre Technology CO. LTD. School of Food and Pharmacy Zhejiang Ocean University

In everyday life, traditional dressings such as band-aid and gauze are used for dealing with small wounds.However, these dressings have shortcomings such as pain caused by tearing, inapplicability to joints, single functionality, and adverse reactions. Therefore, there is a great need for an inexpensive, comfortable, and multifunctional wound dressing. In this study, quaternized chitosan(QCS) with a high degree of substitution(107.84%) was successfully prepared and characterized using ultraviolet–visible(UV–vis) spectroscopy, Fourier transform infrared(FT-IR) spectroscopy, X-ray diffraction(XRD), and proton nuclear magnetic resonance(1H NMR). A series of QCS/F127 thermosensitive hydrogels were prepared by physical cross-linking and used as potential wound dressings. Then the temperature sensitivity, hemostatic ability, antibacterial activity, and sustained drug release effect of the hydrogels were investigated to evaluate their multifunctionality as wound dressings. Finally, the effect of QCS concentration on hydrogel properties was explored. The results show that the composite hydrogels have significant hemostatic, antibacterial, and sustained drug release abilities, and they can be rapidly transformed into a gel state and adhere to skin upon reaching body temperature. In addition, the properties of the hydrogels can be adjusted by varying the concentration of QCS, which allows for the preparation of wound dressings that are responsive to needs. Therefore, multifunctional QCS/F127 hydrogels with temperatureresponse characteristics are of great clinical research value as wound dressings.

关键词： Antibacterial activity Drug delivery Hemostasis thermosensitive hydrogel Wound dressing

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Design and evaluation of chitosan-amino acid thermosensitive hydrogel

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Marine Life Science & Technology 2022年第1期4卷 74-87页

作者： Jianan Tong Huiyun Zhou Jingjing Zhou Yawei Chen Jing Shi Jieke Zhang Xinyu Liang Tianyuan Du Chemical Engineering and Pharmaceutics College Henan University of Science and TechnologyLuoyang471023China College of Pharmacy(Engineering Research Center for Medicine) Harbin University of CommerceHarbin150000China

Chitosan/glycerophosphate thermosensitive hydrogel crosslinked physically was a potential drug delivery carrier;however, long gelation time limits its application. Here, chitosan-amino acid (AA) thermosensitive hydrogels were prepared from chitosan (CS), αβ-glycerophosphate (GP), and L-lysine (Lys) or L-glutamic acid (Glu). The prepared CS-Lys/GP and CS-Glu/GP hydrogel showed good thermosensitivity and could form gels in a short time. The optimal parameters of CS-Lys/GP hydrogel were that the concentration of CS-Lys was 2.5%, the ratio of CS/Lys was 3.5/1.0, the ratio of CS-Lys/GP was 4.5/1.0. The optimal parameters of CS-Glu/GP hydrogel were that the concentration of CS-Glu was 3.0%, the ratio of CS/Glu was 2.0/1.0, and the ratio of CS-Glu/GP was 4.0/1.5. Chitosan-amino acid (CS-AA) thermosensitive hydrogel had a three-dimensional network structure. The addition of model drug tinidazole (TNZ) had no obvious effect on the structure of hydrogel. The results of infrared spectroscopy showed that there were hydrogen bonds between amino acids and chitosan. In vitro release results showed that CS-Lys/GP and CS-Glu/GP thermosensitive hydrogels had sustained release effects. Thus, the chitosan-amino acid thermosensitive hydrogels hold great potential as a sustained release drug delivery system.

关键词： Chitosan L-Lysine L-Glutamic acid αβ-Glycerophosphate thermosensitive hydrogel In vitro release

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Camptothecin@HMSNs/thermosensitive hydrogel composite for applications in preventing local breast cancer recurrence

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Chinese Chemical Letters 2018年第12期29卷 1819-1823页

作者： Jing Wu Ying Qu Kun Shi Bingyang Chu Yanpeng Jia Xue Xiao Qianjun He Zhiyong Qian Department of Hematology and Research Laboratory of Hematology State Key Laboratory of BiotherapyWest China HospitalSichuan University and Collaborative Innovation Center Department of Gynecology and Obstetrics West China Second University HospitalSichuan University Key Laboratory of Birth Defects and Related Diseases of Women and Children Sichuan UniversityMinistry of Education National-Regional Key Technology Engineering Laboratory for Medical Ultrasound Guangdong Key Laboratory for Biomedical Measurements and Ultrasound ImagingSchool of Biomedical EngineeringShenzhen University

Camptothecin has a strong tumor killing ability for a variety of tumor cells with its special anti-cancer mechanism including the breast cancer. However, because of its infinite hydrophobic property, its clinical application has been greatly limited. Early prevention of loco regional recurrence for the breast cancer is critical for patients who have undergone breast-conserving therapy. In the study,CPT was used for the inhibition of the recurrence after the operation. The hollow mesoporous silica nanoparticles were used as the carrier to improve the hydrophilic property and increase its bioavailability with the high loading capacity. The ability of the cellular uptake and antitumor activity was increased. hydrogel was the ideal carrier for local therapy, so the CPT@HMSNs were loaded into the PLEL thermo sensitive hydrogel to be injected into the tumor sites after the tumor was resected. The recurrence was reduced in the group of CPT-HMSNs-PLEL and the side effect of CPT was decreased. They exhibit distinguished potential as drug carrier for local delivery.

关键词： Camptothecin Hollow mesoporous silica nanoparticles Breast cancer recurrence thermosensitive hydrogel Local delivery

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Engineering of a NIR-activable hydrogel-coated mesoporous bioactive glass scaffold with dual-mode parathyroid hormone derivative release property for angiogenesis and bone regeneration

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Bioactive Materials 2023年第8期26卷 1-13页

作者： Shi Liu Zhengzhe Han Ji-Na Hao Dapeng Zhang Xianglong Li Yuanyuan Cao Jinghuan Huang Yongsheng Li Lab of Low-Dimensional Materials Chemistry Key Laboratory for Ultrafine Materials of Ministry of EducationFrontier Science Center of the Materials Biology and Dynamic ChemistryShanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China Department of Orthopedic Surgery and Shanghai Institute of Microsurgery on Extremities Shanghai Jiao Tong University Affiliated Sixth People’s Hospital600 Yishan RoadShanghai200233PR China Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical EngineeringShihezi UniversityShihezi832003China

Osteogenesis,osteoclastogenesis,and angiogenesis play crucial roles in bone regeneration.Parathyroid hormone(PTH),an FDA-approved drug with pro-osteogenic,pro-osteoclastogenic and proangiogenic capabilities,has been employed for clinical osteoporosis treatment through systemic intermittent administration.However,the successful application of PTH for local bone defect repair generally requires the incorporation and delivery by appropriate carriers.Though several scaffolds have been developed to deliver PTH,they suffer from the weaknesses such as uncontrollable PTH release,insufficient porous structure and low mechanical strength.Herein,a novel kind of NIR-activable scaffold(CBP/MBGS/PTHrP-2)with dual-mode PTHrP-2(a PTH derivative)release capability is developed to synergistically promote osteogenesis and angiogenesis for high-efficacy bone regeneration,which is fabricated by integrating the PTHrP-2-loaded hierarchically mesoporous bioactive glass(MBG)into the N-hydroxymethylacrylamide-modified,photothermal agent-doped,poly(N-isopropylacrylamide)-based thermosensitive hydrogels through assembly process.Upon on/off NIR irradiation,the thermoresponsive hydrogel gating undergoes a reversible phase transition to allow the precise control of on-demand pulsatile and long-term slow release of PTHrP-2 from MBG mesopores.Such NIR-activated dual-mode delivery of PTHrP-2 by this scaffold enables a well-maintained PTHrP-2 concentration at the bone defect sites to continually stimulate vascularization and promote osteoblasts to facilitate and accelerate bone remodeling.In vivo experiments confirm the significant improvement of bone reparative effect on critical-size femoral defects of rats.This work paves an avenue for the development of novel dual-mode delivery systems for effective bone regeneration.

关键词： Parathyroid hormone Dual-mode release thermosensitive hydrogel Angiogenesis Bone regeneration

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MiRNA 24-3p-rich exosomes functionalized DEGMA-modified hyaluronic acid hydrogels for corneal epithelial healing

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Bioactive Materials 2023年第7期25卷 640-656页

作者： Xiaomin Sun Wenjing Song Lijing Teng Yongrui Huang Jia Liu Yuehai Peng Xiaoting Lu Jin Yuan Xuan Zhao Qi Zhao Yingni Xu Jingjie Shen Xiaoyun Peng Li Ren School of Materials Science and Engineering South China University of TechnologyGuangzhou510006China National Engineering Research Center for Tissue Restoration and Reconstruction Guangzhou510006China Key Laboratory of Biomedical Engineering of Guangdong Province South China University of TechnologyGuangzhou510006China Key Laboratory of Biomedical Materials and Engineering of the Ministry of Education South China University of TechnologyGuangzhou510006China Innovation Center for Tissue Restoration and Reconstruction South China University of TechnologyGuangzhou 510006China School of Biological Science and Engineering South China University of TechnologyGuangzhou510006China Sino-Singapore International Joint Research Institute Guangzhou510555China Bioland Laboratory(Guangzhou Regenerative Medicine and Health Guangdong Laboratory) Guangzhou510005China School of Biology and Engineering Guizhou Medical UniversityGuiyangGuizhou550025China State Key Laboratory of Ophthalmology Zhongshan Ophthalmic CenterSun Yat-sen UniversityGuangzhou510623China

The damage of corneal epithelium may lead to the formation of irreversible corneal opacities and even blindness.The migration rate of corneal epithelial cells directly affects corneal repair.Here,we explored ocu-microRNA 24-3p(miRNA 24-3p)that can promote rabbit corneal epithelial cells migration and cornea repair.Exosomes,an excellent transport carrier,were exacted from adipose derived mesenchymal stem cells for loading with miRNA 24-3p to prepare miRNA 24-3p-rich exosomes(Exos-miRNA 24-3p).It can accelerate corneal epithelial migration in vitro and in vivo.For application in cornea alkali burns,we further modified hyaluronic acid with di(ethylene glycol)monomethyl ether methacrylate(DEGMA)to obtain a thermosensitive hydrogel,also reported a thermosensitive DEGMA-modified hyaluronic acid hydrogel(THH)for the controlled release of Exos-miRNA 24-3p.It formed a highly uniform and clear thin layer on the ocular surface to resist clearance from blinking and extended the drug-ocular-epithelium contact time.The use of THH-3/Exos-miRNA 24-3p for 28 days after alkali burn injury accelerated corneal epithelial defect healing and epithelial maturation.It also reduced corneal stromal fibrosis and macrophage activation.MiRNA 24-3p-rich exosomes functionalized DEGMA-modified hyaluronic acid hydrogel as a multilevel delivery strategy has a potential use for cell-free therapy of corneal epithelial regeneration.

关键词： miRNA 24-3p Exosome Corneal epithelium Cell migration thermosensitive hydrogel

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Injectable polymeric nanoparticle hydrogel system for long-term anti-inflammatory effect to treat osteoarthritis

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Bioactive Materials 2022年第1期7卷 14-25页

作者： Bo-Bae Seo Youngjoong Kwon Jun Kim Ki Hyun Hong Sung-Eun Kim Hae-Ryong Song Young-Min Kim Soo-Chang Song Center for Biomaterials Korea Institute of Science&TechnologySeoul02792South Korea Division of Bio-Medical Science and Technology KIST SchoolKorea University of Science and TechnologySeoul02792South Korea Department of Orthopedic Surgery and Rare Diseases Institute Korea University Medical College Guro HospitalSeoul08308South Korea

Treatment of osteoarthritis(OA)by administration of corticosteroids is a commonly used method in clinics using anti-inflammatory medicine.Oral administration or intra-articular injection of corticosteroids can reduce the pain and progress of cartilage degeneration,but they are usually insufficient to show local and long-term anti-inflammatory effects because of their fast clearance in the body.In this study,we suggest an injectable anti-OA drug depot system for sustained drug release that provides long-term effective therapeutic advantages.Amphiphilic poly(organophosphazene),which has temperature-dependent nanoparticle forming and sol-gel transition behaviors when dissolved in aqueous solution,was synthesized for triamcinolone acetonide(TCA)delivery.Because hydrophobic parts of the polymer can interact with hydrophobic parts of the TCA,the TCA was encapsulated into the self-assembled polymeric nanoparticles.The TCA-encapsulated polymeric nanoparticles(TePNs)were well dispersed in an aqueous solution below room temperature so that they can be easily injected as a sol state into an intra-articular region.However,the TePNs solution transforms immediately to a viscose 3D hydrogel like a synovial fluid in the intra-articular region via the conducted body temperature.An in vitro TCA release study showed sustained TCA release for six weeks.One-time injection of the TePN hydrogel system in an early stage of OA-induced rat model showed a great inhibition effect against further OA progression.The OA-induced knees completely recovered as a healthy cartilage without any abnormal symptoms.

关键词： thermosensitive hydrogel Triamcinolone acetonide Polymer nanoparticle Osteoarthritis Sustained release

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