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hydrogel platform with tunable stiffness based on magnetic nanoparticles cross-linked GelMA for cartilage regeneration and its intrinsic biomechanism

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生物活性材料(英文) 2023年第7期25卷 615-628页

作者： Chenchen Zhou Chunli Wang Kang Xu Zhixing Niu Shujuan Zou Demao Zhang Zhiyong Qian Jinfeng Liao Jing Xie State Key Laboratory of Oral Diseases National Clinical Research Center for Oral DiseasesWest China Hospital of StomatologySichuan UniversityChengdu610041China State Key Laboratory of Biotherapy State Key Laboratory and Collaborative Innovation Center of BiotherapyWest China HospitalSichuan UniversityChengdu610041SichuanChina "111"Project Laboratory of Biomechanics and Tissue Repair Bioengineering CollegeChongqing UniversityChongqing400044China College of Pharmacy Hubei University of Chinese MedicineWuhan430065China Department of Cardiology and Endodontics West China Hospital of StomatologySichuan UniversityChengduSichuan610064China

Cartilage injury affects numerous individuals,but the efficient repair of damaged cartilage is still a problem in clinic.hydrogel is a potent scaffold candidate for tissue regeneration,but it remains a big challenge to improve its mechanical property and figure out the interaction of chondrocytes and stiffness.Herein,a novel hybrid hydrogel with tunable stiffness was fabricated based on methacrylated gelatin(GelMA)and iron oxide nanoparticles(Fe_(2)O_(3))through chemical bonding.The stiffness of Fe_(2)O_(3)/GelMA hybrid hydrogel was controlled by adjusting the concentration of magnetic nanoparticles.The hydrogel platform with tunable stiffness modulated its cellular properties including cell morphology,microfilaments and Young’s modulus of chondrocytes.Interestingly,Fe_(2)O_(3)/GelMA hybrid hydrogel promoted oxidative phosphorylation of mitochondria and facilitated catabolism of lipids in chondrocytes.As a result,more ATP and metabolic materials generated for cellular physiological activities and organelle component replacements in hybrid hydrogel group compared to pure GelMA hydrogel.Furthermore,implantation of Fe_(2)O_(3)/GelMA hybrid hydrogel in the cartilage defect rat model verified its remodeling potential.This study provides a deep understanding of the bio-mechanism of Fe_(2)O_(3)/GelMA hybrid hydrogel interaction with chondrocytes and indicates the hydrogel platform for further application in tissue engineering.

关键词： Magnetic nanoparticles hydrogel Chondrocyte Cartilage defect Cellular metabolism

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hydrogel-derived nitrogen-doped porous carbon framework with vanadium nitride decoration for supercapacitors with superior cycling performance

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Journal of Materials Science & Technology 2023年第24期155卷 167-174页

作者： Ziqiang Wu Qian Chen Changdian Li Lili Zhu Yanan Huang Xiaoguang Zhu Xuebin Zhu Yuping Sun Key Laboratory of Materials Physics Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 China University of Science and Technology of China Hefei 230026 China High Magnetic Field Laboratory HFIPS Chinese Academy of Sciences Hefei 230031 China Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China

Transition metal nitrides(TMNs)and their composites with carbon materials hold tremendous potential for supercapacitor(SC)electrodes because of their excellent electronic conductivity and electrochemical activity.However,realizing cycling stable TMN/carbon-based supercapacitors with economically viable and environmentally-friendly approaches remains a significant challenge.Significantly,polyacrylamide(PAM)hydrogel,as a water-soluble linear polymer electrolyte,is expected to be a remarkable candidate precursor for preparing N-doped porous carbon(NPC)due to the high contents of carbon and nitrogen elements.In this study,vanadium nitride(VN)embedded in PAM hydrogel-derived NPC was fabricated successfully via an ammonia-free process.The VN/NPC delivers a high specific capacitance of 198.3 F g^(−1)at a current density of 1 A g^(−1),with a remarkable cycling stability of 107%after 16,000 cycles.The electrochemical performances of VN/NPC compared to bare VN nanoparticles are strongly improved due to the composite structure.Additionally,the VN/NPC-based solid-state symmetric device delivers an excellent energy density of 21.97µWh cm^(−2)at a power density of 0.5 mW cm^(−2),and an outstanding cycling durability of 90.9%after 18,000 cycles.This work paves the way to design metal nitride/porous carbon materials,which also opens up unique horizons for the recovery of hydrogel electrolyte.

关键词： Vanadium nitride Nitrogen-doped porous carbon Polyacrylamide hydrogel Supercapacitor

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A Generic Strategy to Create Mechanically Interlocked Nanocomposite/hydrogel Hybrid Electrodes for Epidermal Electronics

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Nano-Micro Letters 2024年第5期16卷 120-133页

作者： Qian Wang Yanyan Li Yong Lin Yuping Sun Chong Bai Haorun Guo Ting Fang Gaohua Hu Yanqing Lu Desheng Kong College of Engineering and Applied Sciences National Laboratory of Solid State Microstructureand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023People’s Republic of China State Key Laboratory of Analytical Chemistry for Life Science and Jiangsu Key Laboratory of Artificial Functional MaterialsNanjing UniversityNanjing 210023People’s Republic of China College of Chemical Engineering and Technology Engineering Research Center of Seawater Utilization Technology of Ministry of EducationState Key Laboratory of Reliability and Intelligence of Electrical EquipmentHebei University of TechnologyTianjin 300130People’s Republic of China Key Laboratory of Intelligent Optical Sensing and Manipulation Nanjing UniversityNanjing 210093People’s Republic of China

Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.

关键词： Stretchable electronics Epidermal electronics Silver nanowire Conductive nanocomposites hydrogel

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Biological Tissue-Inspired Ultrasoft,Ultrathin,and Mechanically Enhanced Microfiber Composite hydrogel for Flexible Bioelectronics

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Nano-Micro Letters 2023年第9期15卷 175-189页

作者： Qiang Gao Fuqin Sun Yue Li Lianhui Li Mengyuan Liu Shuqi Wang Yongfeng Wang Tie Li Lin Liu Simin Feng Xiaowei Wang Seema Agarwal Ting Zhang i-Lab Nano-X Vacuum Interconnected WorkstationKey Laboratory of Multifunction Nanomaterials and Smart SystemsSuzhou Institute of Nano-Tech and Nano-Bionics(SINANO)Chinese Academy of Sciences(CAS)Suzhou 215123JiangsuPeople’s Republic of China Department of Chemistry Bavarian Center for Battery Technology(BayBatt)Bayreuth Center for Colloids and Interfacesand Bavarian Polymer InstituteMacromolecular Chemistry IIUniversity of BayreuthUniversitätsstrasse 3095440 BayreuthGermany School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefei 230026AnhuiPeople’s Republic of China Center for Excellence in Brain Science and Intelligence Technology Chinese Academy of ScienceShanghai 200031People’s Republic of China

hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.

关键词： Fiber hydrogel Flexible electronics Thin film Electrospinning

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Stretchable and self-healable hydrogel artificial skin

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National Science Review 2022年第7期9卷 43-55页

作者： Bin Xue Hui Sheng Yongqiang Li Lan Li Weishuai Di Zhengyu Xu Linjie Ma Xin Wang Haoting Jiang Meng Qin Zhibo Yan Qing Jiang Jun-Ming Liu Wei Wang Yi Cao National Laboratory of Solid State Microstructures Department of Physics Nanjing University State Key Laboratory of Pharmaceutical Biotechnology Department of Sports Medicine and Adult Reconstructive Surgery Drum Tower Hospital Affiliated to Medical School of Nanjing University Institute for Brain Sciences Nanjing University Chemistry and Biomedicine Innovation Center Nanjing University

hydrogels have emerged as promising materials for the construction of skin-like mechanical sensors.The common design of hydrogel-based artificial skin requires a dielectric sandwiched between two hydrogel layers for capacitive sensing.However,such a planar configuration limits the sensitivity,stretchability and self-healing properties.Here,we report the design of single-layer composite hydrogels with bulk capacitive junctions as mechanical sensors.We engineer dielectric peptide-coated graphene(PCG) to serve as homogenously dispersed electric double layers in hydrogels.Any mechanical motions that alter the microscopic distributions of PCG in the hydrogels can significantly change the overall capacitance.We use peptide self-assembly to render strong yet dynamic interfacial interactions between the hydrogel network and graphene.The resulting hydrogels can be stretched up to 77 times their original length and self-heal in a few minutes.The devices can effectively sense strain and pressure in both air and aqueous environments,providing tremendous opportunities for next-generation iontronics.

关键词： hydrogel capacitive sensor stretchability self-healing self-assembly

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Bone/cartilage targeted hydrogel: Strategies and applications

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生物活性材料(英文) 2023年第5期23卷 156-169页

作者： Hao Zhang Shunli Wu Weikai Chen Yan Hu Zhen Geng Jiacan Su Institute of Translational Medicine Shanghai UniversityShanghai200444China Musculoskeletal Organoid Research Center Shanghai UniversityShanghai200444China School of Medicine Shanghai UniversityShanghai200444China School of Environmental and Chemical Engineering Shanghai UniversityShanghai200444China

The skeletal system is responsible for weight-bearing,organ protection,and movement.Bone diseases caused by trauma,infection,and aging can seriously affect a patient’s quality of life.Bone targeted biomaterials are suitable for the treatment of bone diseases.Biomaterials with bone-targeted properties can improve drug utilization and reduce side effects.A large number of bone-targeted micro-nano materials have been developed.However,only a few studies addressed bone-targeted hydrogel.The large size of hydrogel makes it difficult to achieve systematic targeting.However,local targeted hydrogel still has significant prospects.Molecules in bone/cartilage extracellular matrix and bone cells provide binding sites for bone-targeted hydrogel.Drug delivery systems featuring microgels with targeting properties is a key construction strategy for bone-targeted hydrogel.Besides,injectable hydrogel drug depot carrying bone-targeted drugs is another strategy.In this review,we summarize the bone-targeted hydrogel through application environment,construction strategies and disease applications.We hope this article will provide a reference for the development of bone-targeted hydrogels.We also hope this article could increase awareness of bone-targeted materials.

关键词： Bone Cartilage hydrogel Target therapy Bone disease

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Non-contact optical characterization of negative pressure in hydrogel voids and microchannels

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Frontiers of Optoelectronics 2022年第1期15卷 113-120页

作者： Shihao Xu Xiaowei Liu Zehua Yu Kang Liu MOE Key Laboratory of Hydrodynamic Transients School of Power and Mechanical EngineeringWuhan UniversityWuhan 430072China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China

Negative pressure in water under tension,as a thermodynamic non-equilibrium state,has facilitated the emergence of inno-vative technologies on microfluidics,desalination,and thermal management.However,the lack of a simple and accurate method to measure negative pressure hinders further in-depth understanding of the properties of water in such a state.In this work,we propose a non-contact optical method to quantify the negative pressure in micron-sized water voids of a hydrogel film based on the microscale mechanical deformation of the hydrogel itself.We tested three groups of hydrogel samples with different negative pressure inside,and the obtained results fit well with the theoretical prediction.Furthermore,we demonstrated that this method can characterize the distribution of negative pressure,and can thus provide the possibility of investigation of the flow behavior of water in negative pressure.These results prove this technique to be a promising approach to characterization of water under tension and for investigation of its properties under negative pressure.

关键词： hydrogel Negative pressure Non-contact Optical

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Chitosan@Puerarin hydrogel for accelerated wound healing in diabetic subjects by miR-29ab1 mediated inflammatory axis suppression

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Bioactive Materials 2023年第1期19卷 653-665页

作者： Xiaoling Zeng Baohui Chen Luping Wang Yingxiao Sun Zhao Jin Xuanyong Liu Liping Ouyang Yun Liao Department of Pharmacy Tongren HospitalShanghai Jiao Tong University School of MedicineShanghai200336China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China Hongqiao International Institute of Medicine Shanghai Jiao Tong University School of MedicineShanghai200336China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of Sciences1 Sub-lane XiangshanHangzhou310024China Cixi Center of Biomaterials Surface Engineering Shanghai Institute of CeramicsChinese Academy of SciencesNingbo315300China

Wound healing is one of the major global health concerns in patients with diabetes.Overactivation of pro-inflammatory M1 macrophages is associated with delayed wound healing in diabetes.miR-29ab1 plays a critical role in diabetes-related macrophage inflammation.Hence,inhibition of inflammation and regulation of miR-29 expression have been implicated as new points for skin wound healing.In this study,the traditional Chinese medicine,puerarin,was introduced to construct an injectable and self-healing chitosan@puerarin(C@P)hydrogel.The C@P hydrogel promoted diabetic wound healing and accelerated angiogenesis,which were related to the inhibition of the miR-29 mediated inflammation response.Compared to healthy subjects,miR-29a and miR-29b1 were ectopically increased in the skin wound of the diabetic model,accompanied by upregulated M1-polarization,and elevated levels of IL-1βand TNF-α.Further evaluations by miR-29ab1 knockout mice exhibited superior wound healing and attenuated inflammation.The present results suggested that miR-29ab1 is essential for diabetic wound healing by regulating the inflammatory response.Suppression of miR-29ab1 by the C@P hydrogel has the potential for improving medical approaches for wound repair.

关键词： hydrogel Diabetic skin wound healing Macrophages miR-29ab1

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Multifunctional hydrogel enhances bone regeneration through sustained release of Stromal Cell-Derived Factor-1αand exosomes

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Bioactive Materials 2023年第7期25卷 460-471页

作者： Lang Chen Chenyan Yu Yuan Xiong Kai Chen Pei Liu Adriana C.Panayi Xiufeng Xiao Qian Feng Bobin Mi Guohui Liu Department of Orthopaedics Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430022China Hubei Province Key Laboratory of Oral and Maxillofacial Development and Regeneration Wuhan430022China Department of Physics and Center for Hybrid Nanostructure(CHyN) University of HamburgLuruper Chaussee 149Hamburg 22761HamburgGermany Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering College of Chemistry and Materials ScienceFujian Normal UniversityFuzhouFujian350007China Division of Plastic Surgery Brigham and Women’s HospitalHarvard Medical SchoolBostonMA02215USA Key Laboratory of Biorheological Science and Technology Ministry of Education College of BioengineeringChongqing UniversityChongqing400044China

Fracture nonunion remains a great challenge for orthopedic surgeons.Fracture repair comprises of three phases,the inflammatory,repair and remodeling stage.Extensive advancements have been made in the field of bone repair,including development of strategies to balance the M1/M2 macrophage populations,and to improve osteogenesis and angiogenesis.However,such developments focused on only one or the latter two phases,while ignoring the inflammatory phase during which cell recruitment occurs.In this study,we combined Stromal Cell-Derived Factor-1α(SDF-1α)and M2 macrophage derived exosomes(M2D-Exos)with a hyaluronic acid(HA)-based hydrogel precursor solution to synthesize an injectable,self-healing,adhesive HA@SDF-1α/M2D-Exos hydrogel.The HA hydrogel demonstrated good biocompatibility and hemostatic ability,with the 4%HA hydrogels displaying great antibacterial activity against gram-negative E.coli and gram-positive S.aureus and Methicillin-resistant Staphylococcus aureus(MRSA).Synchronously and sustainably released SDF-1αand M2D-Exos from the HA@SDF-1α/M2D-Exos hydrogel enhanced proliferation and migration of human bone marrow mesenchymal stem cell(HMSCs)and Human Umbilical Vein Endothelial Cells(HUVECs),promoting osteogenesis and angiogenesis both in vivo and in vitro.Overall,the developed HA@SDF-1α/M2D-Exos hydrogel was compatible with the natural healing process of fractures and provides a new modality for accelerating bone repair by coupling osteogenesis,angiogenesis,and resisting infection at all stages.

关键词： hydrogel SDF-1α Macrophage Exosomes Fracture healing

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Recent advances in small-scale hydrogel-based robots for adaptive biomedical applications

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Nano Research 2024年第2期17卷 649-662页

作者： Mingzhe Nie Qilong Zhao Xuemin Du Institute of Biomedical&Health Engineering Shenzhen Institute of Advanced Technology(SIAT)Chinese Academy of Sciences(CAS)Shenzhen 518055China

Small-scale robots,ranging in size from micrometers to centimeters,have gained significant attention in the biomedical field.However,conventional small-scale robots made of rigid materials encounter challenges in adapting themselves to the soft tissues and complicated environments of human body.Compared to the rigid counterpart,small-scale hydrogel-based robots hold great promises due to their tissue-like low modulus,outstanding biocompatibility and accessible stimuli-responsive capabilities.These attributes offer small-scale hydrogel-based robots with multimodal locomotion and reinforced functions,further enhancing the adaptability in manipulation and tasks execution for various biomedical applications.In this review,we present recent advances in small-scale hydrogel-based robots.We first summarize the design principles of small-scale hydrogel-based robots including materials,fabrication techniques and manipulation strategies,then highlighting their upgraded functions and adaptive biomedical applications.Finally,we discuss existing challenges and future perspectives for small-scale hydrogel-based robots.

关键词： small-scale robot hydrogel locomotion multi-function adaptability

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