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The effect of degree of sintering on the structural and mechanical properties of Si3N4-SiO2 glass ceramics
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science.ORCID iD: 0009-0005-3234-5649
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science.ORCID iD: 0000-0001-6663-6536
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science.ORCID iD: 0000-0001-9529-650X
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Applied Material Science.ORCID iD: 0000-0002-7356-3002
2024 (English)In: Ceramics International, ISSN 0272-8842, E-ISSN 1873-3956, Vol. 50, no 17, p. 30690-30698Article in journal (Refereed) Published
Abstract [en]

Silica-based glass ceramics have been extensively used in biomedical applications due to their superior biocompatibility and controllable properties. However, their low mechanical strength limits their application. This could be addressed by optimizing the crystalline phase which determines their final properties. Silicon nitride has attracted attention due to its combination of good mechanical and biological properties. Therefore, to combine the advantage of silica-based glass and silicon nitride ceramic, this study developed a silicon nitridesilicon dioxide (Si3N4-SiO2) glass ceramics. The effects of spark plasma sintering parameters on the structural and mechanical properties of Si3N4-SiO2 glass ceramics were investigated. Full densification was reached at a sintering temperature of 1300 degrees C, a holding time of 10 min and an applied pressure of 80 MPa (relative density = 99.19 %). No silicon oxynitride (Si2N2O) crystalline phase was formed in the sintered glass ceramics, as confirmed by XRD. The interface between the (3-Si3N4 crystalline and amorphous SiO2 was investigated by HRTEM, and the results indicated that an amorphous interfacial oxide was formed at the interface. The mechanical properties increased with increasing sintering temperature, as a result of the increased density. The Si3N4-SiO2 glass ceramics sintered at 1500 degrees C exhibited the highest value of toughness and flexural strength, at 4.6 +/- 0.28 MPa m1/2 and 360 +/- 27 MPa. The indentation cracks observed by SEM showed that the large (3-Si3N4 grains promoted crack deflection, while the equiaxed Si3N4 grains with a lower aspect ratio led to transgranular fracture. The mechanical properties of these Si3N4-SiO2 glass ceramics are comparable to commercial glass ceramics, indicating their promising aspects in biomedical applications.

Place, publisher, year, edition, pages
Elsevier, 2024. Vol. 50, no 17, p. 30690-30698
Keywords [en]
Glass ceramics, Spark plasma sintering, Mechanical properties
National Category
Ceramics and Powder Metallurgical Materials Other Materials Engineering
Identifiers
URN: urn:nbn:se:uu:diva-536370DOI: 10.1016/j.ceramint.2024.05.369ISI: 001280897500001OAI: oai:DiVA.org:uu-536370DiVA, id: diva2:1890777
Funder
Swedish Research Council, 2020-04341Swedish Research Council, 2019-00207Available from: 2024-08-20 Created: 2024-08-20 Last updated: 2025-02-09Bibliographically approved
In thesis
1. High-performance SiO2 matrix glass ceramics
Open this publication in new window or tab >>High-performance SiO2 matrix glass ceramics
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Silica-based glass ceramics are widely used in biomedical applications due to their exceptional biocompatibility and tailorable properties. However, their application is often limited by low mechanical strength, which can be improved by optimizing the crystalline phase that determines their final properties. Silicon nitride (Si3N4) and Zirconia (ZrO2) are particularly appealing ceramics due to their favorable combination of mechanical strength and biological compatibility. In this thesis, the development of two types of glass ceramics, Si3N4-SiO2 and ZrO2-SiO2 glass ceramics is explored to address these challenges by controlling their microstructure and engineering the nanointerfaces between ceramic/ceramic grains and ceramic grain/glass matrix.

In Si3N4-SiO2 glass ceramics, raw powders containing three different Si3N4 contents were prepared. The results showed that the β-Si3N4 crystalline phase is well distributed within the SiO2 matrix. The mechanical properties of the glass ceramics improved with increasing Si3N4 content and increasing sintering temperature, reaching a maximum flexural strength of 452±33 MPa and fracture toughness of 6.4±0.5 MPa∙m1/2 at 70 wt% Si3N4 composition. The highest antibacterial rate against S. epidermidis was observed in the 50SiN samples, at 79%. 

In the ZrO2-SiO2 glass ceramics, the raw powders with varying types (K+, Mg2+, Al3+, Ce4+, and Ta5+) and amounts of dopants were prepared by a modified sol-gel method. TEM results showed the ZrO2 crystals were embedded within the amorphous SiO2 matrix, with Mg2+, Al3+, and Ce4+ ions primarily segregating at the grain boundaries of ZrO2 crystals while K+ and Ta5+ ions mainly dissolved within the grains. The Mg-doped samples showed the highest toughness at 12.39±1.34 MPa∙m1/2, attributed to the enhanced interfacial strength between the dopants and ZrO2 crystals. FEM simulation shows that enhanced interfacial bonding lead to more diffused cracking and dissipating energy compared to the conventional interfacial weakening theory. The antibacterial performance of the ZrO2-SiO2  was improved by nitrogen ion implantation of the surface. The antibacterial rate against S.aureus reached 49 ± 24% for samples implanted at fluences of 1×1017 ions/cm².

In conclusion, different SiO2 matrix glass ceramics were developed with enhancing mechanical strength and antibacterial properties. The results indicate that these materials hold significant potential for biomedical applications.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2024. p. 66
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2447
Keywords
glass ceramics; silicon nitride; zirconia; toughness; antibacterial properties; spark plasma sintering
National Category
Materials Engineering Bio Materials
Research subject
Engineering Science with specialization in Materials Science
Identifiers
urn:nbn:se:uu:diva-537936 (URN)978-91-513-2226-1 (ISBN)
Public defence
2024-10-25, 101195 Heinz-Otto Kreiss, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2024-10-03 Created: 2024-09-07 Last updated: 2024-10-03

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Zhou, HuasiPersson, CeciliaEngqvist, HåkanXia, Wei

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