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Mussel-inspired nanozyme catalyzed conductive and self-setting hydrogel for adhesive and antibacterial bioelectronics

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Bioactive Materials 2021年第9期6卷 2676-2687页

作者： Zhanrong Jia Xuanhan Lv Yue Hou Kefeng Wang Fuzeng Ren Dingguo Xu Qun Wang Kelong Fan Chaoming Xie Xiong Lu Key Lab of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu610031SichuanChina National Engineering Research Center for Biomaterials Sichuan UniversityChengdu610064China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhenGuangdong518055China College of Life Science and Biotechnology Mianyang Teachers’CollegeMianyang621006China CAS Engineering Laboratory for Nanozyme Key Laboratory of Protein and Peptide PharmaceuticalsInstitute of BiophysicsChinese Academy of SciencesBeijing100101China Nanozyme Medical Center School of Basic Medical SciencesZhengzhou UniversityZhengzhou450001China

adhesive hydrogels have broad applications ranging from tissue engineering to bioelectronics;however,fabricating adhesive hydrogels with multiple functions remains a challenge.In this study,a mussel-inspired tannic acid chelated-Ag(TA-Ag)nanozyme with peroxidase(POD)-like activity was designed by the in situ reduction of ultrasmall Ag nanoparticles(NPs)with TA.The ultrasmall TA-Ag nanozyme exhibited high catalytic activity to induce hydrogel self-setting without external aid.The nanozyme retained abundant phenolic hydroxyl groups and maintained the dynamic redox balance of phenol-quinone,providing the hydrogels with long-term and repeatable adhesiveness,similar to the adhesion of mussels.The phenolic hydroxyl groups also afforded uniform distribution of the nanozyme in the hydrogel network,thereby improving its mechanical properties and conductivity.Furthermore,the nanozyme endowed the hydrogel with antibacterial activity through synergistic effects of the reactive oxygen species generated via POD-like catalytic reactions and the intrinsic bactericidal activity of Ag.Owing to these advantages,the ultrasmall TA-Ag nanozyme-catalyzed hydrogel could be effectively used as an adhesive,antibacterial,and implantable bioelectrode to detect bio-signals,and as a wound dressing to accelerate tissue regeneration while preventing infection.Therefore,this study provides a promising approach for the fabrication of adhesive hydrogel bioelectronics with multiple functions via mussel-inspired nanozyme catalysis.

关键词： Mussel-inspired nanozyme adhesive hydrogel Conductive hydrogel Antibacterial hydrogel Bioelectronics

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Complex coacervate-derived hydrogel with asymmetric and reversible wet bioadhesion for preventing UV light-induced morbidities

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Bioactive Materials 2023年第12期30卷 62-72页

作者： Xin Peng Yuan Li Menghui Liu Zhuo Li Xuemei Wang Kunyu Zhang Xin Zhao Gang Li Liming Bian Guangdong Provincial Engineering Research Center of Molecular Imaging The Fifth Affiliated HospitalSun Yat-sen UniversityZhuhai519000China Department of Orthopaedics&Traumatology Stem Cells and Regenerative Medicine LaboratoryLi Ka Shing Institute of Health SciencesThe Chinese University ofHong KongPrince of Wales HospitalShatin999077Hong Kong Special Administrative Region School of Biomedical Sciences and Engineering Guangzhou International CampusNational Engineering Research Center for Tissue Restoration and ReconstructionGuangdong Provincial Key Laboratory of Biomedical EngineeringKey Laboratory of Biomedical Materials and Engineering of the Ministry of EducationSouth ChinaUniversity of TechnologyGuangzhou510006PR China Department of Biomedical Engineering The Hong Kong Polytechnic UniversityHong Kong

Protecting the skin from UV light irradiation in wet and underwater environments is challenging due to the weak adhesion of existing sunscreen materials but highly desired.Herein we report a polyethyleneimine/thioctic acid/titanium dioxide(PEI/TA/TiO_(2))coacervate-derived hydrogel with robust,asymmetric,and reversible wet bioadhesion and effective UV-light-shielding ability.The PEI/TA/TiO_(2)complex coacervate can be easily obtained by mixing a PEI solution and TA/TiO_(2)powder.The fluid PEI/TA/TiO_(2)coacervate deposited on wet skin can spread into surface irregularities and subsequently transform into a hydrogel with increased cohesion,thereby establishing interdigitated contact and adhesion between the bottom surface and skin.Meanwhile,the functional groups between the skin and hydrogel can form physical interactions to further enhance bioadhesion,whereas the limited movement of amine and carboxyl groups on the top hydrogel surface leads to low adhesion.Therefore,the coacervate-derived hydrogel exhibits asymmetric adhesiveness on the bottom and top surfaces.Moreover,the PEI/TA/TiO_(2)hydrogel formed on the skin could be easily removed using a NaHCO3 aqueous solution without inflicting damage.More importantly,the PEI/TA/TiO_(2)hydrogel can function as an effective sunscreen to block UV light and prevent UV-induced MMP-9 overexpression,inflammation,and DNA damage in animal skin.The advantages of PEI/TA/TiO_(2)coacervate-derived hydrogels include robust,asymmetric,and reversible wet bioadhesion,effective UV light-shielding ability,excellent biocompatibility,and easy preparation and usage,making them a promising bioadhesive to protect the skin from UV light-associated damage in wet and underwater environments.

关键词： adhesive hydrogel Coacervate Asymmetric adhesion Reversible adhesion

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Robust hydrogel adhesives for emergency rescue and gastric perforation repair

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Bioactive Materials 2023年第1期19卷 703-716页

作者： Jing Yu Yanyang Qin Yuxuan Yang Xiaodan Zhao Zixi Zhang Qiang Zhang Yaqiong Su Yanfeng Zhang Yilong Cheng School of Chemistry Xi’an Jiaotong UniversityXi’an710049China Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research College of StomatologyXi’an Jiaotong UniversityXi’an710049China Department of Dermatology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’an Jiaotong UniversityXi’an710061China

Development of biocompatible hydrogel adhesives with robust tissue adhesion to realize instant hemorrhage control and injury sealing,especially for emergency rescue and tissue repair,is still challenging.Herein,we report a potent hydrogel adhesive by free radical polymerization of N-acryloyl aspartic acid(AASP)in a facile and straightforward way.Through delicate adjustment of steric hindrance,the synergistic effect between interface interactions and cohesion energy can be achieved in PAASP hydrogel verified by X-ray photoelectron spectroscopy(XPS)analysis and simulation calculation compared to poly(N-acryloyl glutamic acid)(PAGLU)and poly(N-acryloyl amidomalonic acid)(PAAMI)hydrogels.The adhesion strength of the PAASP hydrogel could reach 120 kPa to firmly seal the broken organs to withstand the external force with persistent stability under physiological conditions,and rapid hemostasis in different hemorrhage models on mice is achieved using PAASP hydrogel as physical barrier.Furthermore,the paper-based Fe^(3+)transfer printing method is applied to construct PAASP-based Janus hydrogel patch with both adhesive and non-adhesive surfaces,by which simultaneous wound healing and postoperative anti-adhesion can be realized in gastric perforation model on mice.This advanced hydrogel may show vast potential as bio-adhesives for emergency rescue and tissue/organ repair.

关键词： adhesive hydrogel Hydrogen bond Amino acid Emergency rescue Gastric perforation repair

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adhesive hydrogels in osteoarthritis:from design to application

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Military Medical Research 2023年第5期10卷 652-679页

作者： Wang-Lin Duan Li-Ning Zhang Raghvendra Bohara Sergio Martin-Saldana Fei Yang Yi-Yang Zhao Yong Xie Ya-Zhong Bu Abhay Pandit Institute of Medical Engineering Department of BiophysicsSchoolof Basic Medical SciencesHealth Science CenterXi’an JiaotongUniversityXi’an 710061China Department of Rehabilitation Medicine the First Medical CenterChinese PLA General HospitalNo.28 Fuxing RoadHaidian DistrictBeijing 100853China CURAM SFI Research Centre for Medical DevicesUniversity of GalwayGalway H91 TK33Ireland Beijing National Laboratory for Molecular Sciences State Key Laboratoryof Polymer Physics and ChemistryInstitute of ChemistryChineseAcademy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academyof SciencesBeijing 100049China Department of Orthopedics the Fourth Medical CenterChinese PLAGeneral HospitalBeijing 100853China National Clinical Research Center for Orthopedics Sports Medicineand RehabilitationBeijing 100853China

Osteoarthritis(OA)is the most common type of degenerative joint disease which affects 7%of the global population and more than 500 million people worldwide.One research frontier is the development of hydrogels for OA treatment,which operate either as functional scaffolds of tissue engineering or as delivery vehicles of functional additives.Both approaches address the big challenge:establishing stable integration of such delivery systems or implants.adhesive hydrogels provide possible solutions to this challenge.However,few studies have described the current advances in using adhesive hydrogel for OA treatment.This review summarizes the commonly used hydrogels with their adhesion mechanisms and components.Additionally,recognizing that OA is a complex disease involving different biological mechanisms,the bioactive therapeutic strategies are also presented.By presenting the adhesive hydrogels in an interdisciplinary way,including both the fields of chemistry and biology,this review will attempt to provide a comprehensive insight for designing novel bioadhesive systems for OA therapy.

关键词： adhesive hydrogel Osteoarthritis Functional additives Cartilage regeneration Interdisciplinary therapy

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Catch bond-inspired hydrogels with repeatable and loading rate-sensitive specific adhesion

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Bioactive Materials 2023年第3期21卷 566-575页

作者： Zuoying Yuan Xiaocen Duan Xing Su Zhuoling Tian Anqi Jiang Zhuo Wan Hao Wang Pengfei Wei Bo Zhao Xiaozhi Liu Jianyong Huang Department of Mechanics and Engineering Science College of EngineeringPeking UniversityBeijing100871China Beijing Innovation Centre for Engineering Science and Advanced Technology Peking UniversityBeijing100871China Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing100871China Department of Biomedical Engineering College of Future TechnologyPeking UniversityBeijing100871China Beijing Biosis Healing Biological Technology Co. LtdBeijing102600China Tianjin Key Laboratory of Epigenetics for Organ Development of Premature Infants Fifth Central Hospital of TianjinTianjin300450China

Biological receptor-ligand adhesion governed by mammalian cells involves a series of mechanochemical pro-cesses that can realize reversible,loading rate-dependent specific interfacial bonding,and even exhibit a counterintuitive behavior called catch bonds that tend to have much longer lifetimes when larger pulling forces are applied.Inspired by these catch bonds,we designed a hydrogen bonding-meditated hydrogel made from acrylic acid-N-acryloyl glycinamide(AA-NAGA)copolymers and tannic acids(TA),which formed repeatable specific adhesion to polar surfaces in an ultra-fast and robust way,but hardly adhered to nonpolar materials.It demonstrated up to five-fold increase in shear adhesive strength and interfacial adhesive toughness with external loading rates varying from 5 to 500 mm min^(-1).With a mechanochemical coupling model based on Monte Carlo simulations,we quantitatively revealed the nonlinear dependence of rate-sensitive interfacial adhesion on external loading,which was in good agreement with the experimental data.Likewise,the developed hydrogels were biocompatible,possessed antioxidant and antibacterial properties and promoted wound healing.This work not only reports a stimuli-responsive hydrogel adhesive suitable for multiple biomedical applications,but also offers an innovative strategy for bionic designs of smart hydrogels with loading rate-sensitive specific adhesion for various emerging areas including flexible electronics and soft robotics.

关键词： adhesive hydrogel Specific adhesion Receptor-ligand interaction Mechanochemical coupling model

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adhesive cryogel particles for bridging confined and irregular tissue defects

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Military Medical Research 2023年第6期10卷 763-777页

作者： Yao-Ting Xue Ming-Yu Chen Jia-Sheng Cao Lei Wang Jia-Hao Hu Si-Yang Li Ji-Liang Shen Xin-Ge Li Kai-Hang Zhang Shu-Qiang Hao Sarun Juengpanich Si-Bo Cheng Tuck-Whye Wong Xu-Xu Yang Tie-Feng Li Xiu-Jun Cai Wei Yang Department of Engineering Mechanics Zhejiang UniversityHang‑zhou 310027China Key Laboratory of Soft Machines and Smart Devices of Zhejiang Province Zhejiang UniversityHangzhou 310027China Center for X‑Mechanics Department of Engineering MechanicsZhejiang Univer‑sityHangzhou 310027China Department of General Surgery Sir Run-Run Shaw HospitalZhejiang UniversityHangzhou 310016China Soft Intelligent Materials Co. LtdSuzhou 215123China School of Biomedical Engineering and Health Sciences and Advanced Membrane Technology Research Centre Universiti Teknologi Malaysia81310 SkudaiMalaysia

Background Reconstruction of damaged tissues requires both surface hemostasis and tissue bridging.Tissues with damage resulting from physical trauma or surgical treatments may have arbitrary surface topographies,making tissue bridging challenging.Methods This study proposes a tissue adhesive in the form of adhesive cryogel particles(ACPs) made from chitosan,acrylic acid,1-ethyl-3-(3-dimethylaminopropyl) carbodiimide(EDC) and N-hydroxysuccinimide(NHS).The adhesion performance was examined by the 180-degree peel test to a collection of tissues including porcine heart,intestine,liver,muscle,and stomach.Cytotoxicity of ACPs was evaluated by cell proliferation of human normal liver cells(LO2)and human intestinal epithelial cells(Caco-2).The degree of inflammation and biodegradability were examined in dorsal subcutaneous rat models.The ability of ACPs to bridge irregular tissue defects was assessed using porcine heart,liver,and kidney as the ex vivo models.Furthermore,a model of repairing liver rupture in rats and an intestinal anastomosis in rabbits were established to verify the effectiveness,biocompatibility,and applicability in clinical surgery.Results ACPs are applicable to confined and irregular tissue defects,such as deep herringbone grooves in the parenchyma organs and annular sections in the cavernous organs.ACPs formed tough adhesion between tissues[(670.9±50.1) J/m^(2) for the heart,(607.6±30.0) J/m^(2) for the intestine,(473.7±37.0) J/m^(2) for the liver,(186.1±13.3) J/m^(2) for the muscle,and(579.3±32.3) J/m^(2) for the stomach].ACPs showed considerable cytocompatibility in vitro study,with a high level of cell viability for 3 d[(98.8±1.2)%for LO2 and(98.3±1.6)%for Caco-2].It has comparable inflammation repair in a ruptured rat liver(P=0.58 compared with suture closure),the same with intestinal anastomosis in rabbits(P=0.40 compared with suture anastomosis).Additionally,ACP-based intestinal anastomosis(less than 30 s) was remarkably faster than the conventional suturing process(more than 10 min).When ACPs

关键词： Tissue reconstruction Wet adhesion adhesive hydrogel Bioadhesive

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Injectable Self‑Healing adhesive pH‑Responsive hydrogels Accelerate Gastric Hemostasis and Wound Healing

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Nano-Micro Letters 2021年第5期13卷 118-134页

作者： Jiahui He Zixi Zhang Yutong Yang Fenggang Ren Jipeng Li Shaojun Zhu Feng Ma Rongqian Wu Yi Lv Gang He Baolin Guo Dake Chu Department of Gastroenterology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anPeople’s Republic of China Frontier Institute of Science and Technology and State Key Laboratory for Mechanical Behavior of MaterialsXi’an Jiaotong UniversityXi’an 710049China Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research College of StomatologyXi’an Jiaotong UniversityXi’an 710049People’s Republic of China Department of Dermatology The First Affiliated Hospital of Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China National Local Joint Engineering Research Center for Precision Surgery and Regenerative Medicine and Surgical Engineering Research Center of Shaanxi Province First Affiliated Hospital of Xi’an Jiaotong UniversityXi’anPeople’s Republic of China Department of Experimental Surgery Xijing HospitalFourth Military Medical UniversityXi’anPeople’s Republic of China Department of Pathology Tangdu HospitalFourth Military Medical UniversityXi’anPeople’s Republic of China

Endoscopic mucosal resection(EMR)and endoscopic submucosal dissection(ESD)are well-established therapeutics for gastrointestinal neoplasias,but complications after EMR/ESD,including bleeding and perforation,result in additional treatment morbidity and even threaten the lives of patients.Thus,designing biomaterials to treat gastric bleeding and wound healing after endoscopic treatment is highly desired and remains a challenge.Herein,a series of injectable pH-responsive selfhealing adhesive hydrogels based on acryloyl-6-aminocaproic acid(AA)and AA-g-N-hydroxysuccinimide(AA-NHS)were developed,and their great potential as endoscopic sprayable bioadhesive materials to efficiently stop hemorrhage and promote the wound healing process was further demonstrated in a swine gastric hemorrhage/wound model.The hydrogels showed a suitable gelation time,an autonomous and efficient self-healing capacity,hemostatic properties,and good biocompatibility.With the introduction of AA-NHS as a micro-cross-linker,the hydrogels exhibited enhanced adhesive strength.A swine gastric hemorrhage in vivo model demonstrated that the hydrogels showed good hemostatic performance by stopping acute arterial bleeding and preventing delayed bleeding.A gastric wound model indicated that the hydrogels showed excellent treatment effects with significantly enhanced wound healing with type I collagen deposition,α-SMA expression,and blood vessel formation.These injectable self-healing adhesive hydrogels exhibited great potential to treat gastric wounds after endoscopic treatment.

关键词： Injectable self-healing hydrogel adhesive hydrogel Gastric hemostasis Gastric wound healing Endoscopic treatment

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