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A polyphenol-modified chitosan hybrid hydrogel with enhanced antimicrobial and antioxidant activities for rapid healing of diabetic wounds

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Nano Research 2023年第1期16卷 905-916页

作者： Zejun Xu Guiting liu Li Zheng Jun Wu The State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan UniversityChengdu 610065China Guangdong Provincial Key Laboratory of Malignant Tumor Epigenetics and Gene Regulation Sun Yat-Sen Memorial HospitalSun Yat-sen UniversityGuangzhou 510120China Guangxi Engineering Center in Biomedical Materials for Tissue and Organ Regeneration Life Science InstitutesGuangxi Medical UniversityNanning 530021China Collaborative Innovation Centre of Regenerative Medicine and Medical BioResource Development and Application Co-constructed by the Province and Ministry Guangxi Medical UniversityNanning 530021China Bioscience and Biomedical Engineering Thrust The Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400China Division of Life Science The Hong Kong University of Science and TechnologyHong Kong 999077China

High oxidative stress injury and bacterial infection are the main challenges that impair wound healing in diabetic patients.Therefore,a hydrogel with enhanced antimicrobial and antioxidant properties was developed for rapid healing of diabetic wounds.In this study,chitosan methacrylate-gallic acid(CSMA-GA)polymer with antioxidant activity,antimicrobial activity,and ultraviolet(UV)-triggered gelling properties was developed as a hydrogel precursor.Meanwhile,amphiphilic Pluronic F127 molecules were used to load hydrophobic chlorhexidine drug molecules to obtain F127/chlorhexidine nanoparticle(NP)with strong antibacterial activity.Subsequently,F127/chlorhexidine NPs were encapsulated in CSMA-GA hydrogel to further enhance its antibacterial activity.The hybrid hydrogel platform(CSMA-GA/F127/chlorhexidine(CMGFC))exhibited high antibacterial efficiency(>99.9%)and strong reactive oxygen species(ROS)scavenging ability(>80.0%),which effectively protected cells from external oxidative stress(upregulated superoxide dismutase(SOD)and glutathione/oxidized glutathione disulfide(GSH/GSSG)levels and downregulated malondialdehyde(MDA)levels).Moreover,in vivo results proved that the CMGFC hydrogel significantly reduced inflammatory responses(downregulated interleukin-6(IL-6)and upregulated interleukin-10(IL-10)levels),promoted angiogenesis(upregulated vascular endothelial growth factor(VEGF)and platelet endothelial cell adhesion molecule-1(CD 31)levels),and wound healing(enhanced collagen deposition and tissue remodelling).Overall,the CMGFC hydrogel with enhanced antimicrobial and antioxidant properties demonstrated significant potential to enhance diabetic wound healing.

关键词： antimicrobial antioxidant diabetic wound hydrogel

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A novel hydrogel with glucose-responsive hyperglycemia regulation and antioxidant activity for enhanced diabetic wound repair

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Nano Research 2022年第6期15卷 5305-5315页

作者： Zejun Xu Guiting liu Qing Li Jun Wu School of Biomedical Engineering Sun Yat-sen UniversityShenzhen 518107China Guangdong Provincial Key Laboratory of Malignant Tumor Epigenetics and Gene Regulation Sun Yat-sen Memorial Hospital Sun Yat-sen UniversityGuangzhou 510120China The State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan UniversityChengdu 610065China School and Hospital of Stomatology Cheeloo College of MedicineShandong UniversityJinan 250012China

Enhanced diabetic wound repair remained a global challenge.Herein,we reported a novel hydrogel with glucose-responsive hyperglycemia regulation and antioxidant activity for enhanced diabetic wound repair.In this study,gallic acid(GA)with strong antioxidant activity was grafted onto chitosan(CS)chains by one-step synthesis,and then incorporated into poly(ethylene glycol)diacrylate(PEG-DA)hydrogel matrix to obtain a novel antioxidant hybrid hydrogel(PEG-DA/CS-GA).Meanwhile,polyethyleneimine(PEI)was modified with a unique glucose-sensitive phenylboronic acid(PBA)molecule to load insulin(PEIPBA/insulin nano-particles,PEI-PBA/insulin NPs),which could be immobilized in the PEG-DA/CS-GA hybrid hydrogel by the formation of dynamic borate bond between the phenylboronic acid groups on the PEI-PBA and the polyphenol groups on the CSGA.The results indicated that the PEG-DA/PEI-PBA/insulin/CS-GA(PPIC)hydrogel platform not only had remarkable biocompatibility,but also displayed extraordinary antioxidant properties(DPPH scavenging rate>95.0%),and effectively protected cells from oxidative damage(decreased MDA levels,increased Superoxide dismutase(SOD)levels and stable GSH/GSSG levels).Meanwhile,the PPIC hydrogel also exhibited unique glucose-responsive insulin release characteristics,and effectively regulated the blood glucose level.The in vitro and in vivo results demonstrated that our PPIC hydrogel could promoted angiogenesis(increased VEGF and CD 31 expression),reshaped the inflammatory microenvironment(decreased IL-6 and increased IL-10 level),and achieved wound closure within 20 days.All these results strongly indicated that the PPIC hydrogel represented a tough and efficient platform for diabetic wound treatment.

关键词： diabetic wound glucose responsive antioxidation hyperglycemia regulation insulin

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Injectable baicalin/F127 hydrogel with antioxidant activity for enhanced wound healing

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Chinese Chemical Letters 2020年第7期31卷 1817-1821页

作者： Guiting liu Ziting Bao Jun Wu Key Laboratory of Sensing Technology and Biomedical Instrument of Guangdong Province School of Biomedical Engineering.Sun Yat-sen UniversityGuangzhou 510006China Research Institute of Sun Yat-sen University in Shenzhen Shenzhen 518057China

Baicalin,extracted from traditional Chinese medicine Scutellaria baicalensis Georg,possesses multiple pharmacological activities and has great potential for chronic skin wound repair.However,the poor solubility and lack of suitable vehicles greatly limit its further application.Herein,we proposed a convenient and robust strategy,employing PBS solution as solvent,to enhance the solubility of baicalin.Furthermore,we constructed injectable baicalin/F127 hydrogels to study their application in skin wound treatment.The composition and temperature sensitivity of baicalin/Pluronic®F-127 hydrogels were confirmed by FTIR and rheological testing,respectively.In vitro release measurement indicated that the first order model was best fitted with the release profile of baicalin from hydrogel matrix.Besides,MTT assay,AO/EO staining assay as well as hemolytic activity test revealed the excellent cytocompatibility of baicalin/F127 hydrogels.Antioxidant activity assay demonstrated the cytoprotective activity of baicalin/F127 hydrogels against reactive oxygen species(ROS).Furthermore,the in vivo experiments exhibited the ability of baicalin/F127 hydrogel to accelerate wound healing.In conclusion,this novel injectable baicalin/F127 hydrogel should have bright application for chronic wound treatment.

关键词： Wound healing Hydrogel Baicalin Antioxidant Injectable

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Tofu as excellent scaffolds for potential bone regeneration

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Chinese Chemical Letters 2020年第12期31卷 3190-3194页

作者： Keqing Huang Guiting liu Zhipeng Gu Jun Wu Key Laboratory of Sensing Technology and Biomedical Instrument of Guangdong Province School of Biomedical EngineeringSun Yat-sen UniversityGuangzhou 510006China Research Institute of Sun Yat-sen University in Shenzhen Shenzhen 518057China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China

Biomimetic scaffolds present the promising potential for bone regeneration.As a natural gel-like traditional food,tofu with porous architecture and proved biological safety indicated a good potential to be a natural scaffold and easy to be improved by surface modification.Hereon,we fabricated the tofubased scaffolds and systematically explored the potential for bone tissue engineering.In addition,the collagen has been introduced by simple coating to further enha nce the surface compatibility of the tofubased scaffold in bone regeneration.The results showed that the tofu-based scaffolds possessed good porous structure and cytocompatibility.Notably,the tofu-based scaffolds could improve the expression of osteogenesis-related genes and proteins,leading to better bone regeneration after 2 months of implantation.All the results indicated that to fu would become an outstanding sustainable natural porous scaffold for bone regeneration with excellent bioactivities.

关键词： Bone regeneration Scaffolds Tofu Collagen Macrophages

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Hyaluronic acid-methacrylic anhydride/polyhexamethylene biguanide hybrid hydrogel with antibacterial and proangiogenic functions for diabetic wound repair

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Chinese Chemical Letters 2022年第12期33卷 5030-5034页

作者： Yike Li Huiyu Zheng Yaxian Liang Ming Xuan Guiting liu Huixu Xie State Key Laboratory of Oral Diseases National Clinical Research Center for Oral DiseasesWest China Hospital of StomatologyState Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610041China

Diabetic wounds lead to a decrease in quality of life and an increase in mortality.Current treatment strategies include preventing bacterial adhesion while improving microcirculation.As a new type of wound dressing that imitates natural skin,hydrogel has gradually emerged with its excellent properties.However,existing hydrogels rarely achieve satisfactory results in promoting wound repair and antibacterial simultaneously.In this case,we prepared methacrylic anhydride chemically modified hyaluronic acid as a hydrogel matrix,added polyhexamethylene biguanide as an antibacterial component,and loaded sodium alginate/salidroside composite microspheres which could sustainably release salidroside and thus promote angiogenesis.Hybrid hydrogel(HAMA/PHMB-Ms)was synthesized via photocrosslinking,and its chemical structure,particle size distribution and microstructure were characterized.The satisfactory antibacterial properties of the HAMA/PHMB(15%)-Ms hydrogel were studied in vitro,and its antibacterial rates against E.coli and S.aureus were 97.85%and 98.56%,respectively.In addition,after demonstrating its good biocompatibility,we verified that the HAMA/PHMB-Ms hydrogel has increased granulation tissue formation,more collagen deposition,more subcutaneous capillary formation,and better wound healing than blank control,HAMA and HAMA/PHMB hydrogel on the back wound model of diabetic mice.The results confirmed that HAMA/PHMB-Ms hydrogel was a promising material for the treatment of the diabetic wounds.

关键词： Hydrogel Diabetic wounds Antibacterial Angiogenesis

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L-Arginine based polyester amide/hyaluronic acid hybrid hydrogel with dual anti-inflammation and antioxidant functions for accelerated wound healing

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Chinese Chemical Letters 2022年第4期33卷 1880-1884页

作者： Tong liu Guiting liu Jianhua Zhang Zhangfan Ding Yike Li Krishna Sigdel Xiaoyi Wang Huixu Xie State Key Laboratory of Oral Diseases National Clinical Research Center for Oral DiseasesDepartment of Head and Neck Oncology SurgeryWest China Hospital of StomatologySichuan UniversityChengdu 610041China The State Key Laboratory of Polymer Materials Engineering Polymer Research Institute of Sichuan UniversityChengdu 610065China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China

Nowadays, there are still many challenges to skin regeneration. As a new type of skin substitute, hydrogel has emerging gradually with its excellent properties. However, it is still a challenge to combine with biological active agents to facilitate skin regeneration. Under the circumstance, we synthesized argininebased poly(ester amide)(Arg-PEA) and hyaluronic acid(HA-MA), and combined them into new hybrid hydrogels via photo-crosslinking. We found that the internal structure and physicochemical properties of hybrid hydrogels were greatly improved with the increase of content of Arg-PEA. Therefore, we designed hybrid hydrogels with 5 wt% and 10 wt% of Arg-PEA content, respectively. Besides, we selected the corresponding anti-inflammatory(CRP, TNF-α) indicators to detect the anti-inflammatory properties of the hybrid hydrogels at the protein level, and the corresponding antioxidant indicators(SOD, GSH/GSSG, MDA)were selected to investigate the antioxidant properties of hybrid hydrogels at the cellular level in vitro.In addition, we also selected relevant genes to test the effect of hybrid hydrogels on fibrosis and vascularization in the process of skin wound healing in vitro and verified them in vivo with a mouse dorsum wound model. The results confirmed that Arg-PEA/HA-MA(AH) hybrid hydrogel was a prospective scaffold material for skin regeneration.

关键词： Hydrogel Skin wound healing Antioxidant Anti-inflammation

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Whole wheat flour coating with antioxidant property accelerates tissue remodeling for enhanced wound healing

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Chinese Chemical Letters 2020年第6期31卷 1612-1615页

作者： Caihong Xian Zhipeng Gu Guiting liu Jun Wu School of Biomedical Engineering Sun Yat-sen UniversityGuangzhou 510006China Research Institute of Sun Yat-Sen University in Shenzhen Shenzhen 518057.China

As a daily food for billions of people for thousands of years,whole grain is rich in phenolic compounds and may have huge potentials to provide natural antioxidants.Herein,owing to the significant biomedical potential,the effect of whole wheat flour solution as antioxidant wound coating for enhanced wound healing has been studied.The results show that the low concentration of whole wheat flour solutions have good biocompatibility and can scavenge radical and intracellular ROS in vitro,accelerating tissue remodeling in vivo to promote wound healing.This kind of whole wheat flour solution has great potential application for cutaneous wound repair.

关键词： Whole wheat flour Coating Antioxidant Tissue remodeling Wound healing

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Progress on intelligent hydrogels based on RAFT polymerization:Design strategy, fabrication and the applications for controlled drug delivery

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Chinese Chemical Letters 2020年第1期31卷 19-27页

作者： Caihong Xian Qijuan Yuan Ziting Bao Guiting liu Jun Wu Key Laboratory of Sensing Technology and Biomedical Instrument of Guangdong Province School of Biomedical EngineeringSun Yat-sen UniversityGuangzhou 510006China Research Institute of Sun Yat-Sen University in Shenzhen Shenzhen 518057China

Although intelligent hydrogels have shown bright potential application in biomedical fields,they were prepared by conventional methods and still face many serious challenges,such as uncontrollable stimulus-response and low response sensitivity.Recently,RAFT polymerization provides a versatile strategy for the fabrication of intelligent hydrogels with improved stimulus-response properties,owing to the ability to efficiently construct hydrogel precursors with well-defined structure,such as block copolymer,graft copolymer,star copolymer.In this review,we summarized the recent progress on intelligent hydrogels based on RAFT polymerization with emphasis on their fabrication strategies and applications for controlled drug delivery.

关键词： timulus-responsive Hydrogel RAFT polymerization Drug controlled release Rapid response

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2D nanomaterials for tissue engineering application

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Nano Research 2020年第8期13卷 2019-2034页

作者： Jingyang Zhang Haolin Chen Meng Zhao Guiting liu Jun Wu Key Laboratory of Sensing Technology and Biomedical Instrument of Guangdong Province School of Biomedical EngineeringSun Yat-sen UniversityGuangzhou510006China Shenzhen Lansi Institute of Artificial Intelligence in Medicine Shenzhen518057China Research Institute of Sun Yat-Sen University in Shenzhen Shenzhen518057China

Recently,tissue engineering has developed into a powerful tool for repairing and reconstructing damaged tissues and organs.Tissue engineering scaffolds play a vital role in tissue engineering,as they not only provide structural support for targeted cells but also serve as templates that guide tissue regeneration and control the tissue structure.Over the past few years,owing to unique physicochemical properties and excellent biocompatibility,various types of two-dimensional(2D)nanomaterials have been developed as candidates for the construction of tissue engineering scaffolds,enabling remarkable achievements in bone repair,wound healing,neural regeneration,and cardiac tissue engineering.These efforts have significantly advanced the development of tissue engineering.In this review,we summarize the latest advancements in the application of 2D nanomaterials in tissue engineering.First,each typical 2D nanomaterial is introduced briefly,followed by a detailed description of its applications in tissue engineering.Finally,the existing challenges and prospects for the future of the application of 2D nanomaterials in tissue engineering are discussed.

关键词： two-dimensional(2D)nanomaterials tissue engineering biomedical applications regeneration multifunctional nanomaterials

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High performance solid-state thermoelectric energy conversion via inorganic metal halide perovskites under tailored mechanical deformation

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Frontiers in Energy 2022年第4期16卷 581-594页

作者： Lifu YAN Lingling ZHAO guiting YANG Shichao liu Yang liu Shangchao LIN National Engineering Research Center of Turbo-Generator Vibration School of Energy and EnvironmentSoutheast UniversityNanjing 210096China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power-SourcesShanghai 200245China Key Laboratory for Power Machinery and Engineering of the Ministry of Education School of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

Solid-state thermoelectric energy conversion devices attract broad research interests because of their great promises in waste heat recycling,space power generation,deep water power generation,and temperature control,but the search for essential thermoelectric materials with high performance still remains a great challenge.As an emerging low cost,solution-processed thermoelectric material,inorganic metal halide perovskites CsPb(I_(1–x)Br_(x))_(3) under mechanical deformation is systematically investigated using the first-principle calculations and the Boltzmann transport theory.It is demonstrated that halogen mixing and mechanical deformation are efficient methods to tailor electronic structures and charge transport properties in CsPb(I_(1–x)Br_(x))_(3) synergistically.Halogen mixing leads to band splitting and anisotropic charge transport due to symmetry-breakinginduced intrinsic strains.Such band splitting reconstructs the band edge and can decrease the charge carrier effective mass,leading to excellent charge transport properties.Mechanical deformation can further push the orbital energies apart from each other in a more controllable manner,surpassing the impact from intrinsic strains.Both anisotropic charge transport properties and ZT values are sensitive to the direction and magnitude of strain,showing a wide range of variation from 20%to 400%(with a ZT value of up to 1.85)compared with unstrained cases.The power generation efficiency of the thermoelectric device can reach as high as approximately 12%using mixed halide perovskites under tailored mechanical deformation when the heat-source is at 500 K and the cold side is maintained at 300 K,surpassing the performance of many existing bulk thermoelectric materials.

关键词： inorganic metal halide perovskites mechanical deformation thermoelectrics first-principle calculations Boltzmann transport theory

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