Acta Biomaterialia
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2023
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IF 9.7
Guangdong Sun,Xiuling He,Meilin Feng,Xia Xu,Jine Chen,Yongqiang Wang
Visible light-induced photocrosslinking techniques have attracted significant attention for their flexibility, controllability, safety, and energy conservation, especially in tissue engineering and biofabrication, compared to UV photocrosslinking. Despite these advantages, current photoinitiators are constrained by various challenges, including inadequate photoinitiation efficiency, low biocompatibility, poor water solubility, and limited compatibility with diverse crosslinking systems. Here, a water-soluble derivative of riboflavin, flavin mononucleotide (FMN − ), was used to assess its potential as an initiator in multiple-photocrosslinking systems, including radical photopolymerization, dityrosine, and ditryptophan coupling crosslinking, under blue light irradiation. Blue light irradiation facilitated an efficient electron transfer reaction between FMN − and persulfate, owing to their suitable spectral compatibility and photoactivity. The resulting oxidizing free radicals and excited triplet state of FMN − served as initiating active species for the multiple-photocrosslinking reactions. The combination of FMN − and potassium persulfate (KPS) exhibited exceptional photoinitiation efficiency for various biomaterials, including silk fibroin, gelatin, poly(ethylene glycol) diacrylate, and carboxymethyl cellulose modified with amino acids. Furthermore, the cytocompatibility of the FMN − /KPS photoinitiator was demonstrated by the survival rates of 3T3-LI fibroblasts encapsulated in it, which exceeded 95 % when compared to a commercial initiator. Statement of significance By introducing persulfate, the photoinitiation efficiency of flavin mononucleotide was significantly improved. The application scenarios of flavin mononucleotide and persulfate combinations were also greatly extended, including radical photopolymerization, dityrosine, diphenylalanine, and ditryptophan coupling crosslinking. Among them, the coupling crosslinking of amino acids (di-phenylalanine, and di-tryptophan) modified carboxymethyl cellulose, to our knowledge, was first reported. The excellent cytocompatibility of cell encapsulation further proved that the combinations of flavin mononucleotide and persulfate have great potential in tissue engineering.
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International Journal of Nanomedicine
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2023
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IF 8
Yuqin Feng,Si Qin,Huarun Li,Yemei Yang,Yushi Zheng,Hongsheng Liu,Wei Yin Yap,Xianyi Zhou,Ju Wen
Background Hydrogel dressings have been used as a crucial method to keep the wound wet and hasten the healing process. Due to safety concerns regarding the gel components, low mechanical adhesiveness, and unsatisfactory anti-inflammatory capacity qualities for practical uses in vivo, leading to the clinical translation of wound dressings is still difficult.Methods A type of composite hydrogel (acrylamide/polyethylene glycol diacrylate/tannic acid, ie, AM/PEGDA/TA) by double bond crosslinking, Schiff base, and hydrogen bond interaction is proposed. The mechanical characteristics, adhesiveness, and biocompatibility of the hydrogel system were all thoroughly examined. Additionally, a full-thickness cutaneous wound model was employed to assess the in vivo wound healing capacity of resulting hydrogel dressings.Results Benefiting the mechanism of multiple crosslinking, the designed composite hydrogels showed significant mechanical strength, outstanding adhesive capability, and good cytocompatibility. Moreover, the hydrogel system also had excellent shape adaptability, and they can be perfectly integrated into the irregularly shaped wounds through a fast in situ forming approach. Additional in vivo tests supported the findings that the full-thickness wound treated with the composite hydrogels showed quicker epithelial tissue regeneration, fewer inflammatory cells, more collagen deposition, and greater levels of platelet endothelial cell adhesion molecule (CD31) expression.Conclusion These above results might offer a practical and affordable product or method of skin wound therapy in a medical context.
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Advanced Healthcare Materials
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2023
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IF 10
Zhongwu Bei,Linghong Zhang,Jianan Li,Qi Tong,Kun Shi,Wen Chen,Yan Yu,Ao Sun,Yang Xu,Jie Liu,Zhiyong Qian
The healing of chronic diabetic wounds is a common and significant challenge in the medical field. Despite extensive efforts, the development of hydrogel dressings with satisfactory functionality remains an ongoing concern. In this study, a multifunctional hydrogel wound dressing (PAN/Ag-PLG) with adhesion, antibacterial, hemostatic, and other properties, which can effectively repair diabetic wounds infected with methicillin-resistant Staphylococcus aureus (MRSA), is presented. The hydrogel dressing is composed of gallic acid (GA)-functionalized polylysine (PL)-reduced silver nanoparticles (Ag-PLG), oxidized hyaluronic acid (OHA), and cross-linked polyacrylic acid grafted with N -hydrosuccinimide ester. Notably, compared to most conventional wound dressing that lack adhesion or are difficult to remove, the prepared hydrogels exhibit excellent adhesion and mild stimulation-triggered detachment. In vitro and in vivo experiments reveal that the PAN/Ag-PLG hydrogel exhibits outstanding biocompatibility and antibacterial properties and promotes diabetic wound repair by reducing oxidative damage and promoting cell migration and angiogenesis. The smart PAN/Ag-PLG hydrogel reported in this study provides an approach for the potential clinical development of painless antibacterial dressings.
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ACS Biomaterials Science & Engineering
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2023
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IF 5.8
Zitong Sun,Huilin Wen,Zhengao Di,Yang Zhang,Shaobin Zhang,Zhiqian Zhang,Jing Zhang,Ziyi Yu
Living materials that combine living cells and synthetic matrix materials have become promising research fields in recent years. While multicellular systems present exclusive benefits in developing living materials over single-cell systems, creating artificial multicellular systems can be challenging due to the difficulty in controlling the multicellular assemblies and the complexity of cell-to-cell interactions. Here, we propose a coculture platform capable of isolating and controlling the spatial distribution of algal-bacterial consortia, which can be utilized to construct photosynthetic living fibers. Through coaxial extrusion-based 3D printing, hydrogel fibers containing bacteria or algae can be deposited into designated structures and further processed into materials with precise geometries. In addition, the photosynthetic living fibers demonstrate a significant synergistic catalytic effect resulting from the immobilization of both bacteria and algae, which effectively optimizes sewage treatment for bioremediation purposes. The integration of microbial consortia and 3D printing yields functional living materials with promising applications in biocatalysis, biosensing, and biomedicine. Our approach provides an optimized solution for constructing efficient multicellular systems and opens a new avenue for the development of advanced materials.
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ACS Biomaterials Science & Engineering
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2023
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IF 5.8
Shubin Chong,Chengxiu Wei,Longbao Feng,Rui Guo
Microneedles have shown great advantages in subcutaneous drug delivery and skin disease treatment. Vitiligo is a difficult-to-cure skin disease characterized by the depigmentation of the epidermis. Melanosomes produced in melanocytes are transported through dendrites to adjacent keratinocytes, where they accumulate, resulting in skin pigmentation. However, melanocytes in vitiligo patients are functionally disrupted. Silk fibroin (SF) methacrylate hydrogel microneedle can deliver α-MSH to the epidermis directly, where α-MSH helps the protection of melanocytes, extension of melanocytic dendrites, and transfer of melanosomes. In addition, the expression of melanogenesis-related melanocyte-inducing transcription factor and tyrosinase-related protein 1 (TRP1) was up-regulated, and the number of hair follicle stem cells increased with good proliferative activity. This slow release α-MSH SF-based hydrogel microneedles provides a new idea for the treatment of vitiligo.
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CHEMISTRY-A EUROPEAN JOURNAL
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2023
·Vol. 29
·期 38
·e202300969
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IF 4.3
Huaqiang Ju,Qing Li Zhu,Min Zuo,Songmiao Liang,Miao Du,Qiang Zheng,Zi Liang Wu
Graphical Tough hydrogels were developed by forming robust hydrazide-Zn 2+ coordination complexes. The mechanical properties of the resultant gels exhibited a notable temperature dependence and thus a good shape-memory ability due to the dynamic nature of coordination bonds. The reactive amine group of the hydrazide enables facile surface modification and functionalization based on Schiff's base reactions. Energy dissipation based on dynamic fracture of metal ligands is an effective way to toughen hydrogels for specific applications in biomedical and engineering fields. Exploration of new kinds of metal-ligand coordinates with robust bonding strength is crucial for the facile synthesis of tough gels. Here a hydrogel toughening strategy based on the formation of robust coordination complexes between the hydrazide ligands and zinc ions is reported. The resultant hydrogels exhibit high strength and toughness at room temperature. Their mechanical properties show temperature dependence due to the dynamic nature of coordination bonds. In addition, the amine group of hydrazides in the gel matrix provides a reactive site for Schiff's base reaction, enabling surface modification without influence on overall mechanical performances of the gel. The hydrazide ligands are easy to synthesize and can coordinate very well with several transition metals. Such a metal-ligand coordination should be suitable to develop tough soft materials with versatile applications.
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Theranostics
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2023
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IF 12.4
Dehong Tan,Wenxiang Zhu,Lujie Liu,Yuanwei Pan,Yangtao Xu,Qinqin Huang,Lingling Li,Lang Rao
Background: Safe and effective wound healing can be a major clinical challenge. Inflammation and vascular impairment are two main causes of inadequate wound healing. Methods: Here, we developed a versatile hydrogel wound dressing, comprising a straightforward physical mixture of royal jelly-derived extracellular vesicles (RJ-EVs) and methacrylic anhydride modified sericin (SerMA), to accelerate wound healing by inhibiting inflammation and promoting vascular reparation. Results: The RJ-EVs showed satisfactory anti-inflammatory and antioxidant effects, and significantly promoted L929 cell proliferation and migration in vitro . Meanwhile, the photocrosslinked SerMA hydrogel with its porous interior structure and high fluidity made it a good candidate for wound dressing. The RJ-EVs can be gradually released from the SerMA hydrogel at the wound site, ensuring the restorative effect of RJ-EVs. In a full-thickness skin defect model, the SerMA/RJ-EVs hydrogel dressing accelerated wound healing with a healing rate of 96.8% by improving cell proliferation and angiogenesis. The RNA sequencing results further revealed that the SerMA/RJ-EVs hydrogel dressing was involved in inflammatory damage repair-related pathways including recombinational repair, epidermis development, and Wnt signaling. Conclusion: This SerMA/RJ-EVs hydrogel dressing offers a simple, safe and robust strategy for modulating inflammation and vascular impairment for accelerated wound healing.
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Bioactive Materials
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2023
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IF 18.9
Gaizhen Kuang,Qingfei Zhang,Yunru Yu,Luoran Shang,Yuanjin Zhao
Prevention of recurrence/metastasis and tissue regeneration are critical for post-surgery treatment of malignant tumors. Here, to address these needs, a novel type of microgel co-loading cryo-shocked cancer cells, immunoadjuvant, and immune checkpoint inhibitor is presented by microfluidic electrospray technology and liquid nitrogen treatment. Owing to the encapsulation of cryo-shocked cancer cells and immunoadjuvant, the microgels can recruit dendritic cells and activate them in situ , and evoke a robust immune response. Moreover, with the combination of the immune checkpoint inhibitor, the antitumor immune response is further enhanced by inhibiting the interaction of PD1 and PDL1. With this, the excellent anti-recurrence and anti-metastasis efficacy of the microgels are demonstrated in an orthotopic breast cancer mouse model. Besides, because of the excellent biocompatibility and appropriate degradation performance, the microgels can provide support for normal cell adhesion and growth, which is beneficial to tissue reconstruction. These properties indicate the great value of the cryo-shocked cancer cell microgels for efficient tumor postoperative combination immunotherapy and tissue regeneration.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Zhe Li,Cong Li,Wei Sun,Yuan Bai,Zhou Li,Yulin Deng
Implantable and wearable transient electronics based on nanogenerators have been applied in self-powered sensing, electrical-stimulation therapy, and other fields. However, the existing devices have a poor ability to match with the shapes of human tissues, and the degradation processes cannot meet individual needs. In this work, a PEGDA/Lap nanocomposite hydrogel was prepared that was based on biocompatible polyglycol diacrylate (PEGDA) and laponite, and a biodegradable single-electrode triboelectric nanogenerator (BS-TENG) was built. The PEGDA/Lap hydrogel has enhanced flexibility and mechanical and electrical performance. Its strain was 1001.8%, and the resistance was 10.8. The composite hydrogel had a good biocompatibility and could effectively promote the adhesion of cells. The BS-TENG could be used as a self-powered device to light an LED and serve as an active sensor for real-time monitoring of breath and various human movements. More importantly, the device could be degraded controllably without any harm. Therefore, BS-TENGs will be mainstream in diagnosis and treatment and play an important role in biomedical science.
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CARBOHYDRATE POLYMERS
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2023
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IF 11.2
Jianqun Wang,Wenxia Xu,Wenxuan Zhang,Junlong Da,Lixue Liu,Xiaowei Huang,Chubo Yang,Yuanbo Zhan,Han Jin,Ying Li,Bin Zhang
Hydrogels are widely used as wound dressings for wound healing, but when hydrogels absorb wound exudate, swelling occurs and compresses the surrounding tissue, affecting healing. A chitosan injectable (CS/4-PA/CAT) hydrogel based on catechol and 4-glutenoic acid was prepared to avoid swelling and promote wound healing. After cross-linking by UV light, pentenyl groups formed hydrophobic alkyl chains which give the hydrogel a hydrophobic network and thus control its swelling. CS/4-PA/CAT hydrogels retained their non-swelling for a long time in PBS solution at 37 °C. CS/4-PA/CAT hydrogels had good injectable and adhesive properties, and had a good killing effect on E. coli and S. aureus and could remove the bacterial biofilms of E. coli and S. aureus . CS/4-PA/CAT hydrogels had good in vitro coagulation function by absorbing red blood cells and platelets. When used in a whole skin injury model, CS/4-PA/CAT-1 hydrogel stimulated fibroblast migration, promoted epithelialization and accelerated collagen deposition to promote defect healing, and showed good hemostatic effects in liver and femoral artery defects in mice. In summary, the non-swelling injectable hydrogel with free radical scavenging, rapid hemostasis, and antibacterial effects would be a promising treatment for defect repair.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Xiong Xueru,Chen Yunhua,Wang Zhenxing,Liu Huan,Le Mengqi,Lin Caihong,Wu Gang,Wang Lin,Shi Xuetao,Jia Yong-Guang,Zhao Yanli
While hydrogels enable a variety of applications in wearable sensors and electronic skins, they are susceptible to fatigue fracture during cyclic deformations owing to their inefficient fatigue resistance. Herein, acrylated β-cyclodextrin with bile acid is self-assembled into a polymerizable pseudorotaxane via precise host-guest recognition, which is photopolymerized with acrylamide to obtain conductive polymerizable rotaxane hydrogels (PR-Gel). The topological networks of PR-Gel enable all desirable properties in this system due to the large conformational freedom of the mobile junctions, including the excellent stretchability along with superior fatigue resistance. PR-Gel based strain sensor can sensitively detect and distinguish large body motions and subtle muscle movements. The three-dimensional printing fabricated sensors of PR-Gel exhibit high resolution and altitude complexity, and real-time human electrocardiogram signals are detected with high repeating stability. PR-Gel can self-heal in air, and has highly repeatable adhesion to human skin, demonstrating its great potential in wearable sensors.
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Gels
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2023
·Vol. 9
·期 4
·302
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IF 4.6
Yazhou Wang,Zhiwei Peng,Dong Zhang,Dianwen Song
Osteoporosis is one of the most disabling consequences of aging, and osteoporotic fractures and a higher risk of subsequent fractures lead to substantial disability and deaths, indicating that both local fracture healing and early anti-osteoporosis therapy are of great significance. However, combining simple clinically approved materials to achieve good injection and subsequent molding and provide good mechanical support remains a challenge. To meet this challenge, bioinspired by natural bone components, we develop appropriate interactions between inorganic biological scaffolds and organic osteogenic molecules, achieving a tough hydrogel that is both firmly loaded with calcium phosphate cement (CPC) and injectable. Here, the inorganic component CPC composed of biomimetic bone composition and the organic precursor, incorporating gelatin methacryloyl (GelMA) and N-Hydroxyethyl acrylamide (HEAA), endow the system with fast polymerization and crosslinking through ultraviolet (UV) photo-initiation. The GelMA-poly (N-Hydroxyethyl acrylamide) (GelMA-PHEAA) chemical and physical network formed in situ enhances the mechanical performances and maintains the bioactive characteristics of CPC. This tough biomimetic hydrogel combined with bioactive CPC is a new promising candidate for a commercial clinical material to help patients to survive osteoporotic fracture.Keywords:injectable hydrogels;osteogenesis;bone cement;biocompatible polymers
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