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JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION · 2022 · IF 3.682

Fabrication of silk fibroin film enhanced by acid hydrolyzed silk fibroin nanowhiskers to improve bacterial inhibition and biocompatibility efficacy

Minjie Lin,Wenjiao Xie,Xiuwen Cheng,Yuncong Yang,Jegatheeswaran Sonamuthu,Ying Zhou,Xiaogang Yang,Yurong Cai

In this study, silk fibroin nanowhiskers (SNWs) were extracted from natural silk fiber by sulfuric acid hydrolysis with the assistance of ultrasonic wave treatment. The obtained SNWs were mixed with regenerated silk fibroin (RSF) solution to fabricate the SNWs/RSF films. The fabricating SNWs were systematically characterized by using SEM, FTIR, and the SNWs/RSF films were observed by digital camera, PM, etc. The results show that the monodisperse SNWs are evenly distributed in the RSF film. The presence of SNWs in RSF film significantly improves the performances of the film, including the swelling ability, mechanical properties, hydrophilicity, antibacterial efficacy, cytocompatibility. Meanwhile, the SNWs/RSF film can endorse the wound healing efficiency in vivo mice wound site. The proposed techniques for extracting SNWs and fabricating silk fibroin composite film may provide a valuable method for creating an ideal silk-based material for biomedical applications.

研究领域: 生物材料学 · 医学工程 · 生物医学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

A dialdehyde pullulan cross-linking strategy for immobilizing protamine onto silk fiber surfaces to achieve durable antibacterial function

Pirah Ayaz,Xi Liu,Yuyun Yu,Shuangfei Xiang,Shujun Zhao,Feiya Fu,Hongyan Diao,Xiangdong Liu

Covalent immobilization of antibacterial peptides (APs) onto silk protein-based materials has always been a challenge due to the lack of green and efficient macromolecular cross-linkers. Here, we proposed a dialdehyde polysaccharide cross-linker oxidized from pullulan for grafting a natural AP protamine (PM) onto silk fiber surface through a simple cold pad-batch process. The oxidized pullulan (OP) was linked to silk fiber surface through Schiff reaction and used for mediated cross-linking of PM also via Schiff base linkages. This modification introduced abundant PM guanidine groups on the fiber leading to much-desired antibacterial activity, and considerable improvement in the moisture transfer properties and shade depth. FTIR, XPS, SEM studies confirmed the presence of PM and the cross-linking structure between the polysaccharide and peptides on the fiber surfaces. The antibacterial activity imparted by this process was retained even after 20 washing and 50 rubbing cycles proving versatility and durability. Further, the process did not affect other critical silk properties such as appearance, tensile strength, biological safety, etc. Immobilization of PM onto silk fibers through this novel green polysaccharide cross-linker makes silk more appealing and usable and could also enlighten the attempts of cross-linking other protein materials.

CAS / MDL: 9057-02-7 7790-28-5
研究领域: 材料科学 · 纺织工程
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ACS Biomaterials Science & Engineering · 2023 · IF 5.8

Stabilization and Sustained Release of Fragrances Using Silk-PEG Microspheres

Jianbing Wu,Wenjun Guo,Yongfeng Wang,Jian Liu,Heng Wang,Zhaozhu Zheng,Xiaoqin Wang,David L. Kaplan

Fragrances, which are commonly used in food, textiles, consumer products, and medical supplies, are volatile compounds that require stabilization and controlled release due to their sensitivity to environmental conditions such as light, oxygen, temperature, and humidity. Encapsulation in various material matrices is a desired technique for these purposes, and there is a growing interest in using sustainable natural materials to reduce environmental impact. In this study, fragrance encapsulation in microspheres made from silk fibroin (SF) was investigated. Fragrance-loaded silk fibroin microspheres (Fr-SFMSs) were prepared by adding fragrance/surfactant emulsions to silk solutions, followed by mixing them with polyethylene glycol under ambient conditions. The study investigated eight different fragrances, where citral, beta-ionone, and eugenol showed higher binding affinities to silk than the other five fragrances, resulting in better microsphere formation with uniform sizes and higher fragrance loading (10–30%). Citral-SFMSs showed characteristic crystalline β-sheet structures of SF, high thermal stability (initial weight loss at 255 °C), long shelf life at 37 °C (>60 days), and sustained release (∼30% of citral remained after incubation at 60 °C for 24 h). When citral-SFMSs with different sizes were used to treat cotton fabrics, about 80% of the fragrance remained on the fabrics after one wash, and the duration of release from the treated fabrics was significantly longer than that of control samples treated with citral alone (no microspheres). This method of preparing Fr-SFMSs has potential applications in textile finishing, cosmetics, and the food industry.

研究领域: 材料科学 · 纺织工程 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Bionic wet-adhesive tooth band-aid with bidirectional anchoring to promote dentin remineralization

Jieyu Zhu,Li Zhen,Yuan Gao,Jun Luo,Jianshu Li,Jiaojiao Yang,Jiyao Li

Tooth defects are regarded as “wounds” on the tooth. While remineralization therapies aim to rebuild tooth structures, challenges remain in protecting defects and delivering remineralization templates due to the wet and dynamic oral environment. Drawing from wound dressing, this study intends to construct a tooth dressing for the oral environment. Tannic acid (TA) was screened to crosslink fibroin protein (SF) and form internal anchoring through hydrogen bonding to fabricate a SF-TA (ST) tooth dressing matrix. Assisted by the drainage effect of the SF hydrophobic side chain on the interface, the system forms external anchoring to the tooth surface via phenolic hydroxyl groups and side chains. Notably, the bidirectional anchoring effect can be enhanced by calcium-phosphorus-enriched saliva, ensuring effective wet adhesion in the oral cavity. Loaded with an octuplet repeat of aspartate-serine-serine (8DSS) as a remineralization template, the SF-TA-8DSS (ST-8DSS) “tooth band-aid” maintains strong wet-adhesion to tooth surface under liquid contamination (bursting pressure above 780 mmHg) and delivers 8DSS into dentinal tubules (up to 100 µm over 14 days), promoting dentin remineralization. The proposed tooth band-aid offers an effective strategy for repairing tooth defects, combining mechanical reinforcement and wet adhesion through bidirectional anchoring for sustained mineralization under fluid contamination.

CAS / MDL: 1401-55-4 7550-35-8
研究领域: 牙科学 · 生物材料学 · 口腔医学
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Heliyon · 2024 · IF 3.4

The polycaprolactone and silk fibroin nanofibers with Janus-structured sheaths for antibacterial and antioxidant by loading Taxifolin

Kun Jiao,Maolei Sun,Wenyuan Jia,Yun Liu,Shaoru Wang,Yuheng Yang,Zhihui Dai,Liping Liu,Zhiqiang Cheng,Guomin Liu,Yungang Luo

Electrospinning is a widely recognized method for producing Janus or core-shell nanofibers. In this study, nanofibrous membranes were fabricated through co-axial electrospinning utilizing polycaprolactone (PCL) and silk fibroin (SF) as the Janus shell, and taxifolin (TAX) and SF as the core. The resulting nanofibers had diameters of 816 ± 161 nm and core diameters of 73 ± 5 nm. The morphology and properties of the PCL-SF@SF/TAX nanofibers were subsequently analyzed. The results demonstrated that the nanofibrous membranes achieved physical and chemical characteristics potential for tissue engineering and drug delivery. Specifically, the membranes exhibited a Young's modulus of 9.64 ± 0.29 MPa, a water contact angle of 79.1 ± 1.3°, and a weight loss of 17.3 ± 1.0 % over a period of 28 days. The incorporation of TAX endowed the membranes with antibacterial properties, effectively combating Escherichia coli and Staphylococcus aureus . Furthermore, the membranes demonstrated antioxidant capabilities, with a DPPH radical scavenging efficiency of 38.5 ± 5.6 % and a Trolox-equivalent antioxidant capacity of 0.24 ± 0.01 mM. The release of the antioxidant was sustained over 28 days, following first-order release kinetics. The nanofibrous membranes, referred to as PSST, exhibit promising potential for use as biomaterials, characterized by their antibacterial activity, antioxidant and cytocompatibility.

研究领域: 生物材料学 · 组织工程学 · 药剂学
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Polymers · 2019 ·Vol. 11 ·期 2 ·302 · IF 3.164

Regenerated Antheraea pernyi Silk Fibroin/Poly(N-isopropylacrylamide) Thermosensitive Composite Hydrogel with Improved Mechanical Strength

Boxiang Wang,Song Zhang,Yifan Wang,Bo Si,Dehong Cheng,Li Liu,Yanhua Lu

At present,Antheraea pernyisilk fibroin (ASF) has attracted research efforts to investigate it as a raw material for fabrication of biomedical devices because of its superior cytocompatibility. Nevertheless, native ASF is not easily processed into a hydrogel without any crosslinking agent, and a single hydrogel shows poor mechanical properties. In this paper, a series of ASF/poly (N-isopropylacrylamide) (PNIPAAm) composite hydrogels with different ASF contents were manufactured by a simple in situ polymerization method without any crosslinking agent. Meanwhile, the structures, morphologies and thermal properties of composite hydrogels were investigated by XRD, FTIR, SEM, DSC and TGA, respectively. The results indicate that the secondary structure of silk in the composite hydrogel can be controlled by changing the ASF content and the thermal stability of composite hydrogels is enhanced with an increase in crystalline structure. The composite hydrogels showed similar lower critical solution temperatures (LCST) at about 32 °C, which matched well with the LCST of PNIPAAm. Finally, the obtained thermosensitive composite hydrogels exhibited enhanced mechanical properties, which can be tuned by varying the content of ASF. This strategy to prepare an ASF-based responsive composite hydrogel with enhanced mechanical properties represents a valuable route for developing the fields of ASF, and, furthermore, their attractive applications can meet the needs of different biomaterial fields.Keywords:Antheraea pernyi;silk fibroin;hydrogel;thermosensitive;mechanical properties

CAS / MDL: 2210-25-5
研究领域: 生物材料学 · 高分子化学 · 组织工程学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2020 · IF 6.155

Silk microfibrous mats with long-lasting antimicrobial function

Mi Wu,Wen Liu,Jinrong Yao,Zhengzhong Shao,Xin Chen

The controlled release of antibiotic drugs to injured sites has great advantages over the conventional intravenous administration of antibiotics, which is associated with systemic toxicity, for wound care. Electrospun nanofibrous/microfibrous mats, with a similar structure to the native extracellular matrix, is a promising wound dressing. Herein, drug-loaded halloysite nanotubes (HNTs) incorporated into regenerated silk fibroin (RSF) microfibrous mats were prepared by electrospinning to achieve sustained drug release and long-lasting antimicrobial protection. A broad-spectrum antibiotic, tetracycline hydrochloride (TCH), was selected as the model drug. Transmission electron microscopic images revealed that the TCH-loaded HNTs were homogeneously embedded in the RSF electrospun microfibers without significant changes in morphology. The drug release profiles showed that the RSF microfibrous mats with TCH-loaded HNTs exhibited a significantly reduced burst phase and a long release time over two weeks compared to the pure TCH-loaded HNTs and the TCH-loaded RSF microfibrous mats without HNTs. These results were attributed to the two-step release of TCH first from the HNTs and then RSF matrix in the electrospun mats. Finally, the antimicrobial properties of the RSF microfibrous mats with TCH-loaded HNTs were evaluated using both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli bacteria. The results demonstrated long-lasting antimicrobial activity for at least one week, showing the great potential of TCH-loaded RSF microfibrous mat as a wound dressing material. Therefore, these TCH-loaded RSF microfibrous mats with excellent biocompatibility and sustained antimicrobial protection are extremely attractive systems for clinical applications.

CAS / MDL: 2231-57-4
研究领域: 生物材料学 · 医学 · 药剂学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2018 · IF 3.909

Preparation of a multifunctional fibroin-based biomaterial via laccase-assisted grafting of chitooligosaccharide

Qian Zhou,Li Cui,Lamei Ren,Ping Wang,Chao Deng,Qiang Wang,Xuedong Fan

Chitooligosaccharide (COS) has the characteristic of antioxidant and antibacterial effects. To improve the properties of silk fibroin (SF), COS was enzymatically grafted onto SF membranes using a laccase from Trametes versicolor . d -Glucosamine hydrochloride (GAH) and p -hydroxyphenylacetamide (PHAD), as the model compound of COS and tyrosine residues in SF were utilized to disclose the grafting mechanism, respectively. The data from UPLC-TQD and GPC analysis implied that laccase might catalyze the oxidation of PHAD and led to the formation of self-polymerized products. FTIR and 1 H NMR results verified the occurrence of the laccase-assisted reactions between COS and PHAD. For the fibroin samples with different treatments, incubation with laccase alone led to remarkable increase in the molecular weight of SF, mainly owing to the efficient self-crosslinks of the fibroin chains. For the COS-grafted SF membrane, there was no obvious change in the thermal behavior, while the antioxidant and antibacterial properties were evidently improved when compared to that of the untreated. Meanwhile, biocompatibility of the COS grafted SF membrane was acceptable according to the cell viability of NIH/3T3 cells. The present work provides a novel method for preparation of the multifunctional fibroin-based biomaterials.

CAS / MDL: 66-84-2
研究领域: 生物材料学 · 酶工程 · 医学材料
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Polymers · 2022 ·Vol. 14 ·期 18 ·3875 · IF 4.967

Electrospinning Silk Fibroin/Graphene Nanofiber Membrane Used for 3D Wearable Pressure Sensor

Zulan Liu,Jiaxuan Wang,Qian Zhang,Zheng Li,Zhi Li,Lan Cheng,Fangyin Dai

With the improvement of science and technology, flexible sensors have become a hot research topic. Flexible sensors have broad application in human health detection and motion detection and other fields. In this paper, the silk fibroin/graphene nanofiber membranes were prepared by double needle electrospinning. In addition, the high sensitivity of the three-dimensional composite hierarchy was obtained by superimposing a monolayer silk fibroin/graphene nanofiber membrane, which was prepared via double needle electrospinning. In addition, the three-dimensional hierarchy was encapsulated by polydimethylsiloxane to prepare a pressure sensor. The sensitivity of the pressure sensor can achieve 7.7 Pa−1. In addition, this pressure sensor has excellent durability (>2000 cycles) and shorter response times (490 ms), which has broad research prospects in human health detection and motion detection.Keywords:silk fibroin;graphene;flexible sensor;electrospinning

研究领域: 材料科学 · 生物医学工程
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Multifunctional and durable thermal management coating from sericin-MXene biohybrid on silk fabric micro-etched by deep eutectic solvent

Haiwei Yang,Lvzhu Cheng,Qiliang Yang,Amjad Farooq,Lili Ying,Peng Wang,Zongqian Wang

Integration of natural textiles ( e.g. silk) and two-dimensional transition metal carbide/nitride (MXene) is promising for the development of wearable thermal management materials. However, fabricating MXene-decorated textiles with durable and stable thermal management performance remains a challenge due to the susceptible oxidation of MXene and the weak interaction between MXene and fibers. Here, we propose a novel surface modification strategy for MXene nanosheets (SSMXene) by co-assembling with natural sericin to protect against water and oxygen, enrich surface chemistry, and significantly enhance oxidative stability. Subsequently, SSMXene-coated silk fabrics (M-silk) were developed via choline chloride/oxalic acid deep eutectic solvent (DES) micro-etching pretreatment and then decorating SSMXene through a scalable solution dip-coating technique. Notably, DES micro-etching pretreatment enabled strong interfacial bonding between SSMXene and fibers through the synergistic effect of hydrogen bonding and mechanical locking. The fabricated M-silk not only demonstrated desirable thermal management performance, including active electrical heating (the maximum temperature rise = 55.6 °C) and passive radiative heating (the mid-infrared emissivity as low as 0.24 at 7–14 μm), but also possessed superior breathability, laundry durability, and flame retardancy. Therefore, the smart, comfortable, durable, and multifunctional M-silk displays great potential for achieving effective personal thermal management.

研究领域: 材料科学 · 纺织工程
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Journal of Materials Chemistry B · 2019 ·Vol. 7 ·期 9 ·1450-1459 · IF 5.047

Preparation of natural amphoteric silk nanofibers by acid hydrolysis

Yanlei Hu,Juan Yu,Liang Liu,Yimin Fan

Direct extraction of silk nanofibers (SNs) from natural silk fibers was developed via a low-intensity ultrasonic-assisted sulfuric acid hydrolysis process. The effects of sulfuric acid (H2SO4) amount, hydrolysis time and temperature were investigated. SNs with a length and width of 306 ± 107 nm and 4–18 nm, respectively, were obtained with a yield of 64.54%. Furthermore, unlike for the silk nanofibers formed from a regeneration process, the original crystal structure of the silk was maintained. The aqueous dispersion of SNs was steady for at least 30 days at pH 3 and 7–10 with no aggregation. Furthermore, the as-prepared SNs were amphoteric due to the intrinsic characteristics of the protein that endow them with the ability to mix well with either positively or negatively charged polymers, possibly contributing to the field of high-tech silk materials in the future.

研究领域: 材料科学 · 生物化学
✓ 已验证 DOI PubMed 高影响因子
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Silk fibroin microneedles loaded with melatonin for circadian rhythm regulation

Xiaoyue Li,Yanai Chen,Huiyan Shao,Zheng Yan,Yun Wang,Shenzhou Lu

As a new type of transdermal drug delivery preparation, microneedles can improve the bioavailability of drugs and enhance patient compliance. This article develops a melatonin transdermal sustained-release microneedles using silk fibroin as the substrate. The silk fibroin in microneedles forms a SILK I crystal structure, which does not dissolve in the skin but has certain swelling properties. Microneedles have superior mechanical properties, and can puncture the skin to form a sustained-release channel in the dry state. After drug release is completed, wet microneedles can be pulled out. The results of in vitro transdermal experiments show that the effective drug release time of microneedles is significantly correlated with drug loading. The sustained release time of melatonin silk fibroin microneedles with a drug loading of 1 mg/tablet reach 11 h, with a cumulative release rate of over 85 %. The results of in vivo animal experiments show that silk fibroin melatonin microneedles can maintain a stable blood drug concentration for up to 8 h. The results of in vivo pharmacodynamics show that melatonin microneedles have significant therapeutic effects on insomnia model rats, improving disrupted circadian rhythms and alleviating anxiety.

研究领域: 药剂学 · 生物医学工程 · 药物递送系统
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