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Protein-Based Composite Materials

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Macromolecules".

Deadline for manuscript submissions: closed (31 August 2022) | Viewed by 18562

Special Issue Editor

Special Issue Information

Dear Colleagues,

A protein composite is a material system with two or more macro/micro/nano constituents of different shapes, properties or chemical compositions, at least one of which is a protein. Typical protein polymers include animal proteins (e.g., silk, keratin, collagen, elastin, resilin, reflectin), plant proteins (e.g., corn zein, soy, wheat gluten), as well as their related protein peptides derived from recombinant biotechnology. Compared to synthetic polymers, proteins have the advantages of being biocompatible, biodegradable, and sustainable with tunable mechanical strength and water solubility. The design of multifunctional and tunable protein-based composite materials is an emerging area of research, with a wide range of applications in the booming biomedical device/green material/biomaterial industry, including tissue regeneration, drug delivery, antibody and vaccine storage, disease models, flexible biosensors, green plastics, biophotonics, and nano-biotechnology.

By optimizing molecular interfaces between different components, protein-based composite materials can be fabricated into a variety of materials, such as particles, fibers, films, gels, or sponges, and encompass a range of functions, such as thermal conductivity at different temperatures, elasticity to support diverse structures, electromagnetic sensitivity in variable sensors, and optical properties for advanced biotechnology.

The aim of this Special Issue is to discuss their design, synthesis, characterization, manufacturing or modeling, as well as their various physical and chemical applications in the biomedical and green industry fields. We cordially invite you to contribute to the themed issue. Both original research and review articles are welcome.

Dr. Xiao Hu
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

  • Protein biopolymer
  • Composite film, fiber, foam, gel, particle, sensor, and device
  • Biomacromolecules and functional materials
  • Polymer composite design and characterization
  • Protein physical and chemical properties

Published Papers (7 papers)

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Research

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24 pages, 7290 KiB  
Article
Novel Amoxicillin-Loaded Sericin Biopolymeric Nanoparticles: Synthesis, Optimization, Antibacterial and Wound Healing Activities
by Shaimaa E. Diab, Nourhan A. Tayea, Bassma H. Elwakil, Abir Abd El Mageid Gad, Doaa A. Ghareeb and Zakia A. Olama
Int. J. Mol. Sci. 2022, 23(19), 11654; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms231911654 - 01 Oct 2022
Cited by 6 | Viewed by 2292
Abstract
Infected wounds are a major threat among diabetic patients. Technological advancements are currently increasing the number of new adjunctive therapies that may be potent agents for speeding recovery, lowering the amputation rate and limiting infection recurrences. A novel formula with promising antibacterial activity, [...] Read more.
Infected wounds are a major threat among diabetic patients. Technological advancements are currently increasing the number of new adjunctive therapies that may be potent agents for speeding recovery, lowering the amputation rate and limiting infection recurrences. A novel formula with promising antibacterial activity, namely sericin/propolis/Amoxicillin nanoparticles, was assessed as a potent treatment of infected wounds in normal and diabetic rats. Skin wound healing efficiency was assessed through wound healing scorings, bacterial load assessment and histological examinations. It was revealed that upon using sericin/propolis/Amoxicillin nanoparticles, complete wound healing was successfully achieved after 10 and 15 days postinjury for nondiabetic and diabetic rats, respectively. However, the bacterial load in the induced infected wounds was extremely low (0–10 CFU/mL) after 15 days post-treatment. The histological studies revealed that the dermis was more organized with new matrix deposition, and mature collagen fibers were observed among the treated animal groups. The present study is the first preclinical study which reported the importance of silk sericin in the form of nano-sericin/propolis loaded with Amoxicillin as an effective treatment against bacterial wound infections. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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13 pages, 2995 KiB  
Article
Removal of Copper(II) from Aqueous Environment Using Silk Sericin-Derived Carbon
by Yuting Xiao, Ruixiao Luo, Yansong Ji, Shiwei Li, Hongmei Hu and Xiaoning Zhang
Int. J. Mol. Sci. 2022, 23(19), 11202; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms231911202 - 23 Sep 2022
Cited by 3 | Viewed by 1479
Abstract
Sericin is a by-product of the silk industry. Its recycling contributes to environmental protection and the sustainable development of the cocoon silk industry. In this paper, on the basis of realizing sericin enrichment in solution, the Cu(II) adsorption capacities of sericin-derived carbon (SC), [...] Read more.
Sericin is a by-product of the silk industry. Its recycling contributes to environmental protection and the sustainable development of the cocoon silk industry. In this paper, on the basis of realizing sericin enrichment in solution, the Cu(II) adsorption capacities of sericin-derived carbon (SC), prepared at different pyrolysis temperatures, were studied. SC was characterized using scanning electron microscopy (SEM) and the zeta potential. The effects of the initial concentration of Cu(II), pH, adsorption temperature, and contact time on the adsorption process were evaluated, followed by an investigation of the mechanism of Cu(II) adsorption by SC. The results showed that SC has a porous structure that provides sites for Cu(II) adsorption. The maximum adsorption capacity of Cu(II) onto SC1050, 17.97 mg/g, was obtained at an adsorption temperature of 35 °C and a pH of 5.5. In addition, the pseudo-second-order kinetic model and Langmuir isotherm model correctly described the adsorption process of Cu(II) onto SC1050. Therefore, SC can act as a potential adsorbent for removing Cu(II) from water. This study helps promote the effective use of cocoon silk resources. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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17 pages, 4785 KiB  
Article
Silk/Rayon Webs and Nonwoven Fabrics: Fabrication, Structural Characteristics, and Properties
by Yu Jeong Bae, Mi Jin Jang and In Chul Um
Int. J. Mol. Sci. 2022, 23(14), 7511; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms23147511 - 06 Jul 2022
Cited by 7 | Viewed by 1724
Abstract
Silk is a naturally occurring material and has been widely used in biomedical and cosmetic applications owing to its unique properties, including blood compatibility, excellent cytocompatibility, and a low inflammatory response in the body. A natural silk nonwoven fabric with good mechanical properties [...] Read more.
Silk is a naturally occurring material and has been widely used in biomedical and cosmetic applications owing to its unique properties, including blood compatibility, excellent cytocompatibility, and a low inflammatory response in the body. A natural silk nonwoven fabric with good mechanical properties was recently developed using the binding property of sericin. In this study, silk/rayon composite nonwoven fabrics were developed to increase productivity and decrease production costs, and the effect of the silk/rayon composition on the structure and properties of the fabric was examined. The crystalline structure of silk and rayon was maintained in the fabric. As the silk content increased, the porosity and moisture regain of the silk/rayon web and nonwoven fabric decreased. As the silk content increased, the maximum stress of the web and nonwoven fabric increased, and the elongation decreased. Furthermore, the silk/rayon web exhibited the highest values of maximum stress and elongation at ~200 °C. Regardless of the silk/rayon composition, all silk/rayon nonwoven fabrics showed good cytocompatibility. Thus, the silk/rayon fabric is a promising material for cosmetic and biomedical applications owing to its diverse properties and high cell viability. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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26 pages, 3079 KiB  
Article
Functional Properties of Two-Component Hydrogel Systems Based on Gelatin and Polyvinyl Alcohol—Experimental Studies Supported by Computational Analysis
by Karolina Labus, Lukasz Radosinski and Piotr Kotowski
Int. J. Mol. Sci. 2021, 22(18), 9909; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22189909 - 14 Sep 2021
Cited by 10 | Viewed by 2323
Abstract
The presented research is focused on an investigation of the effect of the addition of polyvinyl alcohol (PVA) to a gelatin-based hydrogel on the functional properties of the resulting material. The main purpose was to experimentally determine and compare the properties of hydrogels [...] Read more.
The presented research is focused on an investigation of the effect of the addition of polyvinyl alcohol (PVA) to a gelatin-based hydrogel on the functional properties of the resulting material. The main purpose was to experimentally determine and compare the properties of hydrogels differing from the content of PVA in the blend. Subsequently, the utility of these matrices for the production of an immobilized invertase preparation with improved operational stability was examined. We also propose a useful computational tool to predict the properties of the final material depending on the proportions of both components in order to design the feature range of the hydrogel blend desired for a strictly specified immobilization system (of enzyme/carrier type). Based on experimental research, it was found that an increase in the PVA content in gelatin hydrogels contributes to obtaining materials with a visibly higher packaging density, degree of swelling, and water absorption capacity. In the case of hydrolytic degradation and compressive strength, the opposite tendency was observed. The functionality studies of gelatin and gelatin/PVA hydrogels for enzyme immobilization indicate the very promising potential of invertase entrapped in a gelatin/PVA hydrogel matrix as a stable biocatalyst for industrial use. The molecular modeling analysis performed in this work provides qualitative information about the tendencies of the macroscopic parameters observed with the increase in the PVA and insight into the chemical nature of these dependencies. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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18 pages, 23887 KiB  
Article
Synthesis of pH and Glucose Responsive Silk Fibroin Hydrogels
by Xiaosheng Tao, Fujian Jiang, Kang Cheng, Zhenzhen Qi, Vamsi K. Yadavalli and Shenzhou Lu
Int. J. Mol. Sci. 2021, 22(13), 7107; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22137107 - 01 Jul 2021
Cited by 16 | Viewed by 3770
Abstract
Silk fibroin (SF) has attracted much attention due to its high, tunable mechanical strength and excellent biocompatibility. Imparting the ability to respond to external stimuli can further enhance its scope of application. In order to imbue stimuli-responsive behavior in silk fibroin, we propose [...] Read more.
Silk fibroin (SF) has attracted much attention due to its high, tunable mechanical strength and excellent biocompatibility. Imparting the ability to respond to external stimuli can further enhance its scope of application. In order to imbue stimuli-responsive behavior in silk fibroin, we propose a new conjugated material, namely cationic SF (CSF) obtained by chemical modification of silk fibroin with ε-Poly-(L-lysine) (ε-PLL). This pH-responsive CSF hydrogel was prepared by enzymatic crosslinking using horseradish peroxidase and H2O2. Zeta potential measurements and SDS-PAGE gel electrophoresis show successful synthesis, with an increase in isoelectric point from 4.1 to 8.6. Fourier transform infrared (FTIR) and X-ray diffraction (XRD) results show that the modification does not affect the crystalline structure of SF. Most importantly, the synthesized CSF hydrogel has an excellent pH response. At 10 wt.% ε-PLL, a significant change in swelling with pH is observed. We further demonstrate that the hydrogel can be glucose-responsive by the addition of glucose oxidase (GOx). At high glucose concentration (400 mg/dL), the swelling of CSF/GOx hydrogel is as high as 345 ± 16%, while swelling in 200 mg/dL, 100 mg/dL and 0 mg/dL glucose solutions is 237 ± 12%, 163 ± 12% and 98 ± 15%, respectively. This shows the responsive swelling of CSF/GOx hydrogels to glucose, thus providing sufficient conditions for rapid drug release. Together with the versatility and biological properties of fibroin, such stimuli-responsive silk hydrogels have great potential in intelligent drug delivery, as soft matter substrates for enzymatic reactions and in other biomedical applications. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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16 pages, 4962 KiB  
Article
Chemical, Thermal, Time, and Enzymatic Stability of Silk Materials with Silk I Structure
by Meihui Zhao, Zhenzhen Qi, Xiaosheng Tao, Chad Newkirk, Xiao Hu and Shenzhou Lu
Int. J. Mol. Sci. 2021, 22(8), 4136; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms22084136 - 16 Apr 2021
Cited by 38 | Viewed by 3245
Abstract
The crystalline structure of silk fibroin Silk I is generally considered to be a metastable structure; however, there is no definite conclusion under what circumstances this crystalline structure is stable or the crystal form will change. In this study, silk fibroin solution was [...] Read more.
The crystalline structure of silk fibroin Silk I is generally considered to be a metastable structure; however, there is no definite conclusion under what circumstances this crystalline structure is stable or the crystal form will change. In this study, silk fibroin solution was prepared from B. Mori silkworm cocoons, and a combined method of freeze-crystallization and freeze-drying at different temperatures was used to obtain stable Silk I crystalline material and uncrystallized silk material, respectively. Different concentrations of methanol and ethanol were used to soak the two materials with different time periods to investigate the effect of immersion treatments on the crystalline structure of silk fibroin materials. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Raman scattering spectroscopy (Raman), Scanning electron microscope (SEM), and Thermogravimetric analysis (TGA) were used to characterize the structure of silk fibroin before and after the treatments. The results showed that, after immersion treatments, uncrystallized silk fibroin material with random coil structure was transformed into Silk II crystal structure, while the silk material with dominated Silk I crystal structure showed good long-term stability without obvious transition to Silk II crystal structure. α-chymotrypsin biodegradation study showed that the crystalline structure of silk fibroin Silk I materials is enzymatically degradable with a much lower rate compared to uncrystallized silk materials. The crystalline structure of Silk I materials demonstrate a good long-term stability, endurance to alcohol sterilization without structural changes, and can be applied to many emerging fields, such as biomedical materials, sustainable materials, and biosensors. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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Review

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21 pages, 4114 KiB  
Review
Recent Research Progress of Ionic Liquid Dissolving Silks for Biomedicine and Tissue Engineering Applications
by Hang Heng, Qianqian Deng, Yipeng Yang and Fang Wang
Int. J. Mol. Sci. 2022, 23(15), 8706; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms23158706 - 05 Aug 2022
Cited by 8 | Viewed by 2345
Abstract
Ionic liquids (ILs) show a bright application prospect in the field of biomedicine and energy materials due to their unique recyclable, modifiability, structure of cation and anion adjustability, as well as excellent physical and chemical properties. Dissolving silk fibroin (SF), from different species [...] Read more.
Ionic liquids (ILs) show a bright application prospect in the field of biomedicine and energy materials due to their unique recyclable, modifiability, structure of cation and anion adjustability, as well as excellent physical and chemical properties. Dissolving silk fibroin (SF), from different species silkworm cocoons, with ILs is considered an effective new way to obtain biomaterials with highly enhanced/tailored properties, which can significantly overcome the shortcomings of traditional preparation methods, such as the cumbersome, time-consuming and the organic toxicity caused by manufacture. In this paper, the basic structure and properties of SF and the preparation methods of traditional regenerated SF solution are first introduced. Then, the dissolving mechanism and main influencing factors of ILs for SF are expounded, and the fabrication methods, material structure and properties of SF blending with natural biological protein, inorganic matter, synthetic polymer, carbon nanotube and graphene oxide in the ILs solution system are introduced. Additionally, our work summarizes the biomedicine and tissue engineering applications of silk-based materials dissolved through various ILs. Finally, according to the deficiency of ILs for dissolving SF at a high melting point and expensive cost, their further study and future development trend are prospected. Full article
(This article belongs to the Special Issue Protein-Based Composite Materials)
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