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Bioceramic scaffolds with two-step internal/external modification of copper-containing polydopamine enhance antibacterial and alveolar Bone regeneration capability

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Journal of Zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第1期25卷 65-82页

作者： Xiaojian JIANG Lihong LEI Weilian SUN Yingming WEI Jiayin HAN Shuaiqi ZHONG Xianyan YANG Zhongru GOU Lili CHEN Department of Oral Medicine the Second Affiliated HospitalZhejiang University School of MedicineHangzhou310009China Bio-nanomaterials and Regenerative Medicine Research Division Zhejiang–California International Nanosystem InstituteZhejiang UniversityHangzhou310058China

Magnesium-doped calcium silicate(CS)bioceramic scaffolds have unique advantages in mandibular defect repair;however,they lack antibacterial properties to cope with the complex oral microbiome.Herein,for the first time,the CS scaffold was functionally modified with a novel copper-containing polydopamine(PDA(Cu^(2+)))rapid deposition method,to construct internally modified(*P),externally modified(@PDA),and dually modified(*P@PDA)scaffolds.The morphology,degradation behavior,and mechanical properties of the obtained scaffolds were evaluated in vitro.The results showed that the CS*P@PDA had a unique micro-/nano-structural surface and appreciable mechanical resistance.During the prolonged immersion stage,the release of copper ions from the CS*P@PDA scaffolds was rapid in the early stage and exhibited long-term sustained release.The in vitro evaluation revealed that the release behavior of copper ions ascribed an excellent antibacterial effect to the CS*P@PDA,while the scaffolds retained good cytocompatibility with improved osteogenesis and angiogenesis effects.Finally,the PDA(Cu^(2+))-modified scaffolds showed effective early Bone regeneration in a critical-size rabbit mandibular defect model.Overall,it was indicated that considerable antibacterial property along with the enhancement of alveolar Bone regeneration can be imparted to the scaffold by the two-step PDA(Cu^(2+))modification,and the convenience and wide applicability of this technique make it a promising strategy to avoid bacterial infections on implants.

关键词： Copper-containing polydopamine Modification Antibacterial property Bone regeneration Angiogenesis Bioceramic scaffold

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Piezoresistive MXene/Silk fibroin nanocomposite hydrogel for accelerating Bone regeneration by Re-establishing electrical microenvironment

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Bioactive Materials 2023年第4期22卷 1-17页

作者： Zhi-Chao Hu Jia-Qi Lu Tai-Wei Zhang Hai-Feng Liang Hao Yuan Di-Han Su Wang Ding Rui-Xian Lian Yu-Xiang Ge Bing Liang Jian Dong Xiao-Gang Zhou Li-Bo Jiang Department of Orthopaedic Surgery Zhongshan HospitalFudan UniversityShanghai200032China Key Laboratory of Advanced Display and System Applications of Ministry of Education Shanghai UniversityShanghai200072China Department of Orthopedics Surgery Minhang HospitalFudan UniversityShanghai201100China Key Laboratory for Ultrafine Materials of Ministry of Education Frontiers Science Center for Materiobiology and Dynamic ChemistryResearch Center for Biomedical Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China Department of Orthopedic Surgery Zhongshan Hospital(Xiamen)Fudan UniversityXiamen361015China

The electrical microenvironment plays an important role in bone repair.However,the underlying mechanism by which electrical stimulation(ES)promotes Bone regeneration remains unclear,limiting the design of bone microenvironment-specific electroactive materials.Herein,by simple co-incubation in aqueous suspensions at physiological temperatures,biocompatible regenerated silk fibroin(RSF)is found to assemble into nanofibrils with aβ-sheet structure on MXene nanosheets,which has been reported to inhibit the restacking and oxidation of MXene.An electroactive hydrogel based on RSF and bioencapsulated MXene is thus prepared to promote efficient Bone regeneration.This MXene/RSF hydrogel also acts as a piezoresistive pressure transducer,which can potentially be utilized to monitor the electrophysiological microenvironment.RNA sequencing is performed to explore the underlying mechanisms,which can activate Ca^(2+)/CALM signaling in favor of the direct osteogenesis process.ES is found to facilitate indirect osteogenesis by promoting the polarization of M2 macrophages,as well as stimulating the neogenesis and migration of endotheliocytes.Consistent improvements in Bone regeneration and angiogenesis are observed with MXene/RSF hydrogels under ES in vivo.Collectively,the MXene/RSF hydrogel provides a distinctive and promising strategy for promoting direct osteogenesis,regulating immune microenvironment and neovascularization under ES,leading to re-establish electrical microenvironment for Bone regeneration.

关键词： Bone regeneration Electrical microenvironment Regenerated silk fibroin MXene Electrical stimulation

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Promoting lacunar Bone regeneration with an injectable hydrogel adaptive to the microenvironment

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Bioactive Materials 2023年第3期21卷 403-421页

作者： Ao Zheng Xiao Wang Xianzhen Xin Lingjie Peng Tingshu Su Lingyan Cao Xinquan Jiang Department of Prosthodontics Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShanghai Engineering Research Center of Advanced Dental Technology and Materials639 Zhizaoju RoadShanghai200011China

Injectable hydrogel is suitable for the repair of lacunar bone deficiency.This study fabricated an injectable,self-adaptive silk fibroin/mesoporous bioglass/sodium alginate(SMS)composite hydrogel system.With controllable and adjustable physical and chemical properties,the SMS hydrogel could be easily optimized adaptively to different clinical applications.The SMS hydrogel effectively showed great injectability and shapeability,allowing defect filling with no gap.Moreover,the SMS hydrogel displayed self-adaptability in mechanical reinforcement and degradation,responsive to the concentration of Ca2+and inflammatory-like pH value in the microenvi-ronment of bone deficiency,respectively.In vitro biological studies indicated that SMS hydrogel could promote osteogenic differentiation of bone marrow mesenchymal stem cells by activation of the MAPK signaling pathway.The SMS hydrogel also could improve migration and tube formation of human umbilical vein endothelial cells.Investigations of the crosstalk between osteoblasts and macrophages confirmed that SMS hydrogel could regulate macrophage polarization from M1 to M2,which could create a specific favorable environment to induce new bone formation and angiogenesis.Meanwhile,SMS hydrogel was proved to be antibacterial,especially for gram-negative bacteria.Furthermore,in vivo study indicated that SMS could be easily applied for maxillary sinus elevation,inducing sufficient new bone formation.Thus,it is convincing that SMS hydrogel could be potent in a simple,minimally invasive and efficient treatment for the repair of lacunar bone deficiency.

关键词： Injectable hydrogel Oral and maxillofacial Silk fibroin Lacunar bone deficiency Bone regeneration

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3D printed pore morphology mediates bone marrow stem cell behaviors via RhoA/ROCK2 signaling pathway for accelerating Bone regeneration

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Bioactive Materials 2023年第8期26卷 413-424页

作者： Qiji Lu Jingjing Diao Yingqu Wang Jianlang Feng Fansen Zeng Yan Yang Yudi Kuang Naru Zhao Yingjun Wang School of Materials Science and Engineering South China University of TechnologyGuangzhou510641PR China National Engineering Research Center for Tissue Restoration and Reconstruction South China University of TechnologyGuangzhou510006PR China NMPA Key Laboratory for Research and Evaluation of Innovative Biomaterials for Medical Devices.Guangzhou 510006PR China Medical Devices Research&Testing Center of SCUT Guangzhou510006PR China School of Biomedical Sciences and Engineering South China University of TechnologyGuangzhou International CampusGuangzhou511442PR China Guangdong Institute of Advanced Biomaterials and Medical Devices Guangzhou510535PR China

bone bionics and structural engineering have sparked a broad interest in optimizing artificial scaffolds for better Bone regeneration.However,the mechanism behind scaffold pore morphology-regulated Bone regeneration remains unclear,making the structure design of scaffolds for bone repair challenging.To address this issue,we have carefully assessed diverse cell behaviors of bone mesenchymal stem cells(BMSCs)on theβ-tricalcium phosphate(β-TCP)scaffolds with three representative pore morphologies(i.e.,cross column,diamond,and gyroid pore unit,respectively).Among the scaffolds,BMSCs on theβ-TCP scaffold with diamond pore unit(designated as D-scaffold)demonstrated enhanced cytoskeletal forces,elongated nucleus,faster cell mobility,and better osteogenic differentiation potential(for example,the alkaline phosphatase expression level in D-scaffold were 1.5-2 times higher than other groups).RNA-sequencing analysis and signaling pathway intervention revealed that Ras homolog gene family A(RhoA)/Rho-associated kinase-2(ROCK2)has in-depth participated in the pore morphology-mediated BMSCs behaviors,indicating an important role of mechanical signaling transduction in scaffold-cell interactions.Finally,femoral condyle defect repair results showed that D-scaffold could effectively promote endogenous Bone regeneration,of which the osteogenesis rate was 1.2-1.8 times higher than the other groups.Overall,this work provides insights into pore morphology-mediated Bone regeneration mechanisms for developing novel bioadaptive scaffold designs.

关键词： bone mesenchymal stem cells 3D-printed scaffold Pore morphology Bone regeneration Structure-osteogenesis relationship

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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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Multiscale design of stiffening and ROS scavenging hydrogels for the augmentation of mandibular Bone regeneration

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Bioactive Materials 2023年第2期20卷 111-125页

作者： Yanlin Wu Xuan Li Yimin Sun Xiujun Tan Chenglin Wang Zhenming Wang Ling Ye State Key Laboratory of Oral Diseases West China Hospital of StomatologySichuan UniversityChengdu610041China

Although biomimetic hydrogels play an essential role in guiding bone remodeling,reconstructing large bone defects is still a significant challenge since bioinspired gels often lack osteoconductive capacity,robust mechanical properties and suitable antioxidant ability for Bone regeneration.To address these challenges,we first engineered molecular design of hydrogels(gelatin/polyethylene glycol diacrylate/2-(dimethylamino)ethyl methacrylate,GPEGD),where their mechanical properties were significantly enhanced via introducing trace amounts of additives(0.5 wt%).The novel hybrid hydrogels show high compressive strength(>700 kPa),stiff modulus(>170 kPa)and strong ROS-scavenging ability.Furthermore,to endow the GPEGD hydrogels excellent osteoinductions,novel biocompatible,antioxidant and BMP-2 loaded polydopamine/heparin nanoparticles(BPDAH)were developed for functionalization of the GPEGD gels(BPDAH-GPEGD).In vitro results indicate that the antioxidant BPDAH-GPEGD is able to deplete elevated ROS levels to protect cells viability against ROS damage.More importantly,the BPDAH-GPEGD hydrogels have good biocompatibility and promote the osteo differentiation of preosteoblasts and Bone regenerations.At 4 and 8 weeks after implantation of the hydrogels in a mandibular bone defect,Micro-computed tomography and histology results show greater bone volume and enhancements in the quality and rate of Bone regeneration in the BPDAH-GPEGD hydrogels.Thus,the multiscale design of stiffening and ROS scavenging hydrogels could serve as a promising material for Bone regeneration applications.

关键词： Biomimetic hydrogels Multiscale design ROS scavenging Stiffness Bone regeneration

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Functionalize d 3D-printe d porous titanium scaffold induces in situ vascularized Bone regeneration by orchestrating bone microenvironment

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Journal of Materials Science & Technology 2023年第22期153卷 92-105页

作者： Bo Yuan Pin Liu Rui Zhao Xiao Yang Zhanwen Xiao Kai Zhang Xiangdong Zhu Xingdong Zhang National Engineering Research Center for Biomaterials Sichuan UniversityChengdu 610064China College of Biomedical Engineering Sichuan UniversityChengdu 610064China

Titanium(Ti)and its alloys have been extensively explored for treating load-bearing bone defects.How-ever,high-stress shielding,weak osteogenic activity,and insufficient vascularization remain key chal-lenges for the long-term clinical outcomes of Ti-based implants.Herein,inspired by structural and func-tional cues of Bone regeneration,a silicon-doped nano-hydroxyapatite(nSiHA)/titanium dioxide(TiO_(2))composite coating with a hierarchical micro/nano-network structure is constructed on the surface of a 3D-printed porous Ti scaffold via a combined strategy of acid-alkali(AA)treatment and electrochemi-cal deposition technique,which not only endows the scaffold with excellent osteoinduction ability but can also effectively immobilize and release vascular endothelial growth factor(VEGF).The results of the in vitro cell experiments show that the functionalized Ti scaffold significantly promotes osteogenesis in bone marrow mesenchymal stem cells(BMSCs)and angiogenesis in human umbilical vein endothelial cells(HUVECs)by activating the extracellular signal-regulated protein kinase(ERK)and HIF-1αsignaling pathways.After being implanted into a rat femoral condyle defect model,the functionalized Ti scaffold can induce in situ vascularized Bone regeneration by orchestrating the two coupled processes of angio-genesis and osteogenesis.These findings indicate that the functionalized Ti scaffold has great potential in bone tissue regeneration and is a promising candidate for load-bearing bone defect repair.

关键词： Porous titanium 3D-printing Hierarchical micro/nano-structure bone microenvironment Vascularization Bone regeneration

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Metal-Doped Brushite Cement for Bone regeneration

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Journal of Bionic Engineering 2023年第6期20卷 2716-2731页

作者： Muhammad Aqib Aneela Anwar Humayun Ajaz Samina Akbar Ahsan Manzoor Maham Abid Zohaib Waheed Qudsia Kanwal Department of Chemistry University of Engineering and TechnologyGT RoadLahore54890Pakistan Department of Chemistry University of LahoreLahore5400Pakistan

For the past several years,calcium phosphate cement was used in the biomedical applications.Outstanding biocompatibility,good bioactivity,self-setting qualities,minimum setting degree,appropriate toughness,and simple shape to accommodate any difficult geometry are among their most notable attributes.Calcium phosphate has some types and brushite is one of the most attractive mineral for bone repair application.Brushite is extensively employed in filling fractures and trauma treatments as a bone substituted material.This kind of material can potentially be used as a medicine delivery device.The replacement of metal,such as magnesium,zinc,and strontium ions,into the calcium phosphate structure is a major research topic these days.Brushite cement has low mechanical strength and quick setting rate.It is possible to produce biomaterials with higher mechanical characteristics.By adding metal that are great potential in controlling cellular density when included into biomaterials.As a result,it is a successful method to develop quite well regenerative medicine.This paper provides a detailed summary of the present achievements of metal-doped brushite cement for bone repair and healing process.The major purpose of this work is to give a simple but thorough analysis of current successes in brushite cement doped with Zn,Mg,Sr,and other ions as well as to highlight new advancements and prospects.The impact of metal replacement on cement physical and chemical properties,including microstructure,setting time,injectability,mechanical property,and ion release,is explored.The metal-doped cement has osteogenesis,angiogenesis,and antibacterial properties,as well as their prospective utility as drug carriers,also considered.

关键词： Calcium phosphate Brushite bone cement Metal dopants Bone regeneration

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Stratified-structural hydrogel incorporated with magnesium-ion-modified black phosphorus nanosheets for promoting neuro-vascularized Bone regeneration

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Bioactive Materials 2022年第10期7卷 271-284页

作者： Yan Xu Chao Xu Lei He Junjie Zhou Tianwu Chen Liu Ouyang Xiaodong Guo Yanzhen Qu Zhiqiang Luo Deyu Duan Department of Orthopaedics Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430074China College of Life Science and Technology Huazhong University of Science and TechnologyChina Wuhan430022China Department of Pathology Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430022China Fudan University Sports Medicine Institute Shanghai200040China

Angiogenesis and neurogenesis play irreplaceable roles in bone repair.Although biomaterial implantation that mimics native skeletal tissue is extensively studied,the nerve-vascular network reconstruction is neglected in the design of biomaterials.Our goal here is to establish a periosteum-simulating bilayer hydrogel and explore the efficiency of bone repair via enhancement of angiogenesis and neurogenesis.In this contribution,we designed a bilayer hydrogel platform incorporated with magnesium-ion-modified black phosphorus(BP)nanosheets for promoting neuro-vascularized Bone regeneration.Specifically,we incorporated magnesium-ion-modified black phosphorus(BP@Mg)nanosheets into gelatin methacryloyl(GelMA)hydrogel to prepare the upper hydrogel,whereas the bottom hydrogel was designed as a double-network hydrogel system,consisting of two interpenetrating polymer networks composed of GelMA,PEGDA,andβ-TCP nanocrystals.The magnesium ion modification process was developed to enhance BP nanosheet stability and provide a sustained release platform for bioactive ions.Our results demonstrated that the upper layer of hydrogel provided a bionic periosteal structure,which significantly facilitated angiogenesis via induction of endothelial cell migration and presented multiple advantages for the upregulation of nerve-related protein expression in neural stem cells(NSCs).Moreover,the bottom layer of the hydrogel significantly promoted bone marrow mesenchymal stem cells(BMSCs)activity and osteogenic differentiation.We next employed the bilayer hydrogel structure to correct rat skull defects.Based on our radiological and histological examinations,the bilayer hydrogel scaffolds markedly enhanced early vascularization and neurogenesis,which prompted eventual Bone regeneration and remodeling.Our current strategy paves way for designing nerve-vascular network biomaterials for Bone regeneration.

关键词： Angiogenesis Neurogenesis Bone regeneration Hydrogel Black phosphorus

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Bio-inspired dual-adhesive particles from microfluidic electrospray for Bone regeneration

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Nano Research 2023年第4期16卷 5292-5299页

作者： Lei Yang Xiaocheng Wang Yunru Yu Luoran Shang Wei Xu Yuanjin Zhao Department of Rheumatology and Immunology Nanjing Drum Tower HospitalSchool of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Oujiang Laboratory(Zhejiang Lab for Regenerative Medicine Vision and Brain Health)Wenzhou InstituteUniversity of Chinese Academy of SciencesWenzhou 325001China Shanghai Xuhui Central Hospital Zhongshan-Xuhui Hospitaland the Shanghai Key Laboratory of Medical Epigeneticsthe International Colaboratory of Medical Epigenetics and Metabolism(Ministry of Science and Technology)Institutes of Biomedical SciencesFudan UniversityShanghai 200032China Department of Orthopedics Tongren HospitalShanghai Jiao Tong University School of MedicineShanghai 200336China

Bioadhesive hydrogels have demonstrated great potential in Bone regeneration.However,the relatively simple adhesion mechanism and lack of intricate structural design restrict their further applications.Herein,inspired by multiple adhesion mechanisms of pollen particles and marine mussels,we present a novel type of dual-adhesive hydrogel particles fabricated from microfluidic electrospray for Bone regeneration.As the particles are rapidly solidified via liquid nitrogen-assisted cryogelation,they exhibit pollen-mimicking hierarchical porous morphology and gain structure-related adhesion.Besides,the particles are further coated by polydopamine(PDA)to achieve molecular-level adhesion especially to physiological wet surfaces of bone issues.Benefiting from such dual-adhesion mechanisms,the particles can strongly adhere to bone tissue defects,and function as porous scaffolds.Moreover,the dual-adhesive particles can serve as effective vehicles to release key growth factors more than two weeks.In vitro experiments showed that the growth factors-loaden particles have excellent biocompatibility and more significantly promote angiogenesis(~2-fold)and osteogenic differentiation(~3-fold)than control.In vivo experiments indicated that the dual-adhesive particles could significantly enhance Bone regeneration(~4-fold)than control by coupling osteogenesis and angiogenesis effects.Based on these features,the bio-inspired dual-adhesive particles have great potentials for bone repair and wound healing applications.

关键词： microfluidics particles growth factors adhesion Bone regeneration

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