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Silk fibroin hydrogels induced and reinforced by acidic calcium phosphate: A simple way of producing bioactive and drug-loadable composites for biomedical applications
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science.ORCID iD: 0000-0002-2594-0213
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science. (Materials in Medicine Group)ORCID iD: 0000-0001-9529-650X
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science. Sichuan University.ORCID iD: 0000-0001-6830-1633
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2021 (English)In: International Journal of Biological Macromolecules, ISSN 0141-8130, E-ISSN 1879-0003, Vol. 193, p. 433-440Article in journal (Refereed) Published
Abstract [en]

Silk fibroin (SF) hydrogels have attracted extensive interest in biomedical applications due to their biocompatibility and wide availability. However, their generally poor mechanical properties limit their utility. Here, injectable, ready-to-use SF-based composites, simultaneously induced and reinforced by acidic calcium phosphates, were prepared via a dual-paste system requiring no complex chemical/physical treatment. The composite was formed by mixing a monocalcium phosphate monohydrate paste with a β-tricalcium phosphate/SF paste. The conformational transition of SF in an acidic environment forms continuous networks, and the acidic calcium phosphate, brushite and monetite, formed simultaneously in the networks during mixing. The composites displayed a partly elastomeric compression behavior, with mechanical properties increasing with an increasing calcium phosphate and β-sheet content at the lower calcium phosphate contents evaluated (22.2–36.4 wt%). While the stiffness was still relatively low, the materials presented a high elasticity and ductility, and no failure at stresses in the range of failure stresses of trabecular bone. Furthermore, the calcium phosphate confers bioactivity to the material, and the composites with a promising in vitro cell response also showed potential as drug vehicles, using vancomycin as a model drug. These dual-paste systems exhibit potential utility in biomedical applications, such as bone void fillers and drug vehicles.

Place, publisher, year, edition, pages
Elsevier, 2021. Vol. 193, p. 433-440
Keywords [en]
silk fibroin, acidic calcium phosphates, composites, hydrogels, mechanical strength, drug-loadable, brushite, dual-paste system
National Category
Ceramics Composite Science and Engineering
Identifiers
URN: urn:nbn:se:uu:diva-356991DOI: 10.1016/j.ijbiomac.2021.10.160ISI: 000729557900006PubMedID: 34715202OAI: oai:DiVA.org:uu-356991DiVA, id: diva2:1237767
Note

Title in thesis list of papers: Silk fibroin hydrogels induced and reinforced by acidic calcium phosphate – A simple way of producing injectable, bioactive and drug-loadable composites for biomedical applications

Authors in thesis list of papers: Luo, J., Wu, D., Engqvist, H., & Persson, C.

Available from: 2018-08-10 Created: 2018-08-10 Last updated: 2024-01-15Bibliographically approved
In thesis
1. Calcium Phosphate Based Biomaterials for Bone Augmentation
Open this publication in new window or tab >>Calcium Phosphate Based Biomaterials for Bone Augmentation
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Basic (apatite-based) calcium phosphate cements (CPCs), and acidic (brushite and monetite-based) CPCs are used as bone replacement materials because of their bioactivity, mouldability and ability to harden in place. However, their application is limited by their inherent brittleness and difficulties related to their handling. The current thesis aimed to provide solutions to these limitations.

To assess the baseline, the mechanical properties of two promising experimental and two commercially available apatite and brushite cements were investigated. The two experimental CPCs exhibited significantly higher mechanical strengths than the two commercially available ones, warranting further advancement of the former towards clinical use.

The setting reaction of brushite cements was, for the first time, quantitatively studied in the first seconds and minutes, using synchrotron X-ray diffraction. The reaction was found to include a fast nucleation induction period (<9 s), nucleation (<18 s), brushite content increase and setting completion. The effect of the commonly used retardant citric acid – which usually also gives stronger brushite cements - was also evaluated, providing important information for further cement development.  

To overcome complicated usage and short shelf life of acidic CPCs, a ready-to-use acidic CPC was developed by mixing a monocalcium phosphate monohydrate (MCPM) paste and a β-tricalcium phosphate (β-TCP) paste with suitable amounts of citric acid. The CPC showed adequate shelf life, good cohesion and mechanical performance.

To mitigate against the brittle behavior of CPCs, i) poly(vinyl alcohol) fibres were used to reinforce apatite cements, significantly improving the apatite matrix’s toughness and resistance to cracking; ii) injectable, ready-to-use organic-inorganic composites with partly elastomeric compression behavior were designed based on silk fibroin hydrogels and acidic calcium phosphates, and their ability for antibiotic drug delivery was assessed. 

In summary, insights into the functional properties of currently available CPCs as well as the setting process of brushite cements were gained and several new calcium phosphate-based formulations were developed to overcome some of the drawbacks of traditional CPCs. Further studies, in particular of the biological response, are needed to verify the potential of the developed materials for future use in the clinical setting. 

 

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2018. p. 55
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1700
Keywords
bone substitute materials, calcium phosphate cements, apatite, brushite, monetite, setting mechanism, premixed, fibre reinforcement, composite, silk fibroin, mechanical properties
National Category
Ceramics Composite Science and Engineering
Research subject
Engineering Science with specialization in Materials Science
Identifiers
urn:nbn:se:uu:diva-356982 (URN)978-91-513-0399-4 (ISBN)
Public defence
2018-09-28, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
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Supervisors
Available from: 2018-09-05 Created: 2018-08-10 Last updated: 2018-09-10

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Wu, DanEngqvist, HåkanLuo, JunPersson, Cecilia

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