Sol-gel derived silicate-phosphate glass SiO2–P2O5–CaO–TiO2: The effect of titanium isopropoxide on porosity and thermomechanical stability

Kovářík, Tomáš; Bělský, Petr; Křenek, Tomáš; Deshmukh, Kalim; Forejtová, Jana; Medlín, Rostislav; Beneš, Jan; Svoboda, Miloš; Kadlec, Jaroslav; Pola, Michal; Jandová, Věra; Mikysek, Petr; Ilavský, Jan; Stich, Theresia; Docheva, Denitsa; Strejcová, Kateřina; Tišler, Zdeněk

doi:10.1016/j.micromeso.2024.113138

Title: Sol-gel derived silicate-phosphate glass SiO₂–P₂O₅–CaO–TiO₂: The effect of titanium isopropoxide on porosity and thermomechanical stability

Journal Article · 17 April 2024 · Microporous and Mesoporous Materials

DOI: https://doi.org/10.1016/j.micromeso.2024.113138 · OSTI ID:2482045

^[1]; Bělský, Petr ^[1]; Křenek, Tomáš ^[1]; Deshmukh, Kalim ^[1]; Forejtová, Jana ^[1]; Medlín, Rostislav ^[1]; Beneš, Jan ^[1]; Svoboda, Miloš ^[1]; Kadlec, Jaroslav ^[1]; Pola, Michal ^[1]; Jandová, Věra ^[2]; Mikysek, Petr ^[2]; Ilavský, Jan ^[3]; Stich, Theresia ^[4]; Docheva, Denitsa ^[5]; Strejcová, Kateřina ^[6]; Tišler, Zdeněk ^[6]

University of West Bohemia, Pilsen (Czech Republic)
Czech Academy of Sciences (CAS), Prague (Czech Republic)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
University Hospital Regensburg (Germany)
University of West Bohemia, Pilsen (Czech Republic); University Hospital Regensburg (Germany); Julius-Maximilians-University Würzburg (Germany)
Unipetrol Centre for Research and Education (UniCRE), Litvínov (Czech Republic)

Despite of several decades lasting extensive research of bioactive and bioresorbable glasses the systematic parametrization and determination of the key factors affecting porosity and thermomechanical characteristics still remains challenging. Here, we present silica-phosphate glasses, with the composition 70SiO_2^-20P₂O_5^-(10-x)CaO-xTiO₂ (mol%; x = 0, 2.5, 5, and 7.5), prepared by sol -gel method and reinforced by titanium dioxide via titanium isopropoxide (TTIP) incorporation which demonstrated tunable variation of porosity from micro-to macro -region and superb mechanical integrity during the calcination process. The presence of 7.5 mol% TiO₂ promotes dimensional stability up to 1000°C as investigated by thermomechanical analysis. The XRD showed the dominant presence of silicon phosphate [Si(P₂O₇)], titanium phosphate [Ti(P₂O₇)] and calcium phosphates [β-Ca(P₂O₆) and γ- Ca₂(P₂O₇)]. The effect of TiO₂ doping on the multiscale morphology and porosity was investigated by means of SEM, MIP, μCT, N₂ adsorption and USAXS/SAXS. Increasing TiO₂ content leads to the formation of open porosity up to 70vol% and drives the formation of a refined interconnected macroporosity of 2-30 μm. In contrast, mesoporosity with a dominance of 3-6nm pores decreases in all samples with increasing TiO₂ content. USAXS/SAXS revealed an increase in primary particle size with increasing TiO₂ content which is in good agreement with the nitrogen physisorption analysis showing that microporosity decreases with increasing TiO2 content.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2482045

Journal Information:: Microporous and Mesoporous Materials, Journal Name: Microporous and Mesoporous Materials Vol. 374; ISSN 1387-1811

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (59)

A Review of Phosphate and Borate Sol–Gel Glasses for Biomedical Applications Lepry, William C.; Nazhat, Showan N. Advanced NanoBiomed Research, Vol. 1, Issue 3 https://doi.org/10.1002/anbr.202000055	journal	January 2021
Bioactive sol‐gel foams for tissue repair Sepulveda, Pilar; Jones, Julian R.; Hench, Larry L. Journal of Biomedical Materials Research, Vol. 59, Issue 2 https://doi.org/10.1002/jbm.1250	journal	November 2001
Titania-Silica Mixed Oxides Dutoit, D. C. M.; Schneider, M.; Baiker, A. Journal of Catalysis, Vol. 153, Issue 1 https://doi.org/10.1006/jcat.1995.1118	journal	April 1995
Application of electro-spray ionization mass spectrometry for characterization of titanium polyoxoalkoxides in sol-gel processes Soloviev, A.; Søgaard, E. G. Journal of Materials Science, Vol. 41, Issue 18 https://doi.org/10.1007/s10853-006-0160-2	journal	September 2006
The story of Bioglass® Hench, Larry L. Journal of Materials Science: Materials in Medicine, Vol. 17, Issue 11 https://doi.org/10.1007/s10856-006-0432-z	journal	November 2006
Physical and biocompatibility studies of novel titanium dioxide doped phosphate-based glasses for bone tissue engineering applications Abou Neel, E. A.; Knowles, J. C. Journal of Materials Science: Materials in Medicine, Vol. 19, Issue 1 https://doi.org/10.1007/s10856-007-3079-5	journal	July 2007
Sol–gel derived 45S5 bioglass: synthesis, microstructural evolution and thermal behaviour Cacciotti, Ilaria; Lombardi, Mariangela; Bianco, Alessandra Journal of Materials Science: Materials in Medicine, Vol. 23, Issue 8 https://doi.org/10.1007/s10856-012-4667-6	journal	May 2012
Sol–gel reactions of titanium alkoxides and water: influence of pH and alkoxy group on cluster formation and properties of the resulting products Simonsen, Morten E.; Søgaard, Erik G. Journal of Sol-Gel Science and Technology, Vol. 53, Issue 3 https://doi.org/10.1007/s10971-009-2121-0	journal	December 2009
Ultra-Small-Angle X-ray Scattering Instrument at the Advanced Photon Source: History, Recent Development, and Current Status Ilavsky, J.; Zhang, F.; Allen, A. J. Metallurgical and Materials Transactions A, Vol. 44, Issue 1 https://doi.org/10.1007/s11661-012-1431-y	journal	October 2012
Thermal evolution of sol–gel-obtained phosphosilicate solids (SiPO) Massiot, Ph; Centeno, M. A.; Carrizosa, I. Journal of Non-Crystalline Solids, Vol. 292, Issue 1-3 https://doi.org/10.1016/S0022-3093(01)00854-7	journal	November 2001
Phosphate glasses for tissue engineering: Part 1. Processing and characterisation of a ternary-based P2O5–CaO–Na2O glass system Ahmed, I.; Lewis, M.; Olsen, I. Biomaterials, Vol. 25, Issue 3 https://doi.org/10.1016/S0142-9612(03)00546-5	journal	February 2004
Effect of increasing titanium dioxide content on bulk and surface properties of phosphate-based glasses Abou Neel, Ensanya Ali; Chrzanowski, Wojciech; Knowles, Jonathan Campbell Acta Biomaterialia, Vol. 4, Issue 3 https://doi.org/10.1016/j.actbio.2007.11.007	journal	May 2008
Bioactive glass in tissue engineering Rahaman, Mohamed N.; Day, Delbert E.; Sonny Bal, B. Acta Biomaterialia, Vol. 7, Issue 6 https://doi.org/10.1016/j.actbio.2011.03.016	journal	June 2011
Titanium phosphate glass microspheres for bone tissue engineering Lakhkar, Nilay J.; Park, Jeong-Hui; Mordan, Nicola J. Acta Biomaterialia, Vol. 8, Issue 11 https://doi.org/10.1016/j.actbio.2012.07.023	journal	November 2012
Bioactive glass-based materials with hierarchical porosity for medical applications: Review of recent advances Baino, Francesco; Fiorilli, Sonia; Vitale-Brovarone, Chiara Acta Biomaterialia, Vol. 42 https://doi.org/10.1016/j.actbio.2016.06.033	journal	September 2016
Optimising bioactive glass scaffolds for bone tissue engineering Jones, Julian R.; Ehrenfried, Lisa M.; Hench, Larry L. Biomaterials, Vol. 27, Issue 7 https://doi.org/10.1016/j.biomaterials.2005.07.017	journal	March 2006
In vitro bioactivity and gene expression by cells cultured on titanium dioxide doped phosphate-based glasses Abou Neel, Ensanya Ali; Mizoguchi, Toshihide; Ito, Michio Biomaterials, Vol. 28, Issue 19 https://doi.org/10.1016/j.biomaterials.2007.03.018	journal	July 2007
3D multiphasic porous scaffolds of calcium phosphates doping with silicon and magnesium Mata, Nayarit A.; Ros-Tárraga, Patricia; Velasquez, Pablo Boletín de la Sociedad Española de Cerámica y Vidrio, Vol. 61, Issue 5 https://doi.org/10.1016/j.bsecv.2021.03.004	journal	September 2022
Synthesis and properties of TiO2-P2O5 and SiO2-TiO2-P2O5 porous hybrids obtained by templating in highly concentrated emulsions Pérez-Carrillo, L. A.; Vílchez, S.; Mosa, J. Ceramics International, Vol. 42, Issue 16 https://doi.org/10.1016/j.ceramint.2016.09.050	journal	December 2016
Photocatalyic activity of double pore structure TiO 2 /SiO 2 monoliths Chang, Wei; Yan, Leilei Ceramics International, Vol. 43, Issue 8 https://doi.org/10.1016/j.ceramint.2017.01.061	journal	June 2017
Bioactive glasses – When glass science and technology meet regenerative medicine Baino, Francesco Ceramics International, Vol. 44, Issue 13 https://doi.org/10.1016/j.ceramint.2018.05.180	journal	September 2018
Current advances in bone tissue engineering concerning ceramic and bioglass scaffolds: A review Ribas, Renata Guimarães; Schatkoski, Vanessa Modelski; Montanheiro, Thaís Larissa do Amaral Ceramics International, Vol. 45, Issue 17 https://doi.org/10.1016/j.ceramint.2019.07.096	journal	December 2019
Hierarchical porous silica monoliths: A novel class of microreactors for process intensification in catalysis and adsorption Galarneau, Anne; Sachse, Alexander; Said, Bilel Comptes Rendus Chimie, Vol. 19, Issue 1-2 https://doi.org/10.1016/j.crci.2015.05.017	journal	January 2016
Comparison on the TiO2 crystalline phases deposited via dip and spin coating using green sol–gel route Johari, Nur Dalilah; Rosli, Zulkifli Mohd; Juoi, Jariah Mohamad Journal of Materials Research and Technology, Vol. 8, Issue 2 https://doi.org/10.1016/j.jmrt.2019.04.018	journal	April 2019
Physicochemical studies of phosphate based P2O5–Na2O–CaO–TiO2 glasses for biomedical applications Rajendran, V.; Gayathri Devi, A. V.; Azooz, M. Journal of Non-Crystalline Solids, Vol. 353, Issue 1 https://doi.org/10.1016/j.jnoncrysol.2006.08.047	journal	January 2007
Structure, solubility and bioactivity in TiO2-doped phosphate-based bioglasses and glass–ceramics Gayathri Devi, A. V.; Rajendran, V.; Rajendran, N. Materials Chemistry and Physics, Vol. 124, Issue 1 https://doi.org/10.1016/j.matchemphys.2010.06.038	journal	November 2010
Preparation and characterisation of porous silica and silica/titania monoliths for potential use in bone replacement Hertz, Audrey; FitzGerald, Victoria; Pignotti, Enrico Microporous and Mesoporous Materials, Vol. 156 https://doi.org/10.1016/j.micromeso.2012.02.004	journal	July 2012
Technical and commercial progress in the adoption of geopolymer cement Van Deventer, Jannie S. J.; Provis, John L.; Duxson, Peter Minerals Engineering, Vol. 29 https://doi.org/10.1016/j.mineng.2011.09.009	journal	March 2012
Synthesis and in vitro bioactivity of mesoporous bioactive glass scaffolds Shih, C. J.; Chen, H. T.; Huang, L. F. Materials Science and Engineering: C, Vol. 30, Issue 5 https://doi.org/10.1016/j.msec.2010.02.006	journal	June 2010
Bioactive glass scaffolds for bone tissue engineering: state of the art and future perspectives Fu, Qiang; Saiz, Eduardo; Rahaman, Mohamed N. Materials Science and Engineering: C, Vol. 31, Issue 7 https://doi.org/10.1016/j.msec.2011.04.022	journal	October 2011
Synthesis of 45S5 Bioglass® via a straightforward organic, nitrate-free sol–gel process Rezabeigi, Ehsan; Wood-Adams, Paula M.; Drew, Robin A. L. Materials Science and Engineering: C, Vol. 40 https://doi.org/10.1016/j.msec.2014.03.042	journal	July 2014
Investigation of bioactivity, biocompatibility and thermal behavior of sol–gel silica glass containing a high PEG percentage Catauro, M.; Renella, R. A.; Papale, F. Materials Science and Engineering: C, Vol. 61 https://doi.org/10.1016/j.msec.2015.11.077	journal	April 2016
Sol–gel based materials for biomedical applications Owens, Gareth J.; Singh, Rajendra K.; Foroutan, Farzad Progress in Materials Science, Vol. 77 https://doi.org/10.1016/j.pmatsci.2015.12.001	journal	April 2016
Small Angle X-ray Scattering for Nanoparticle Research Li, Tao; Senesi, Andrew J.; Lee, Byeongdu Chemical Reviews, Vol. 116, Issue 18 https://doi.org/10.1021/acs.chemrev.5b00690	journal	April 2016
Titanium-Containing Silicate-Based Sol–Gel Bioactive Glass: Development, Characterization, and Applications Smith, Sophia; ElKashty, Osama; Tamimi, Faleh Langmuir, Vol. 37, Issue 49 https://doi.org/10.1021/acs.langmuir.1c01593	journal	December 2021
Preparation of CaO@TiO₂–SiO₂ Biomaterial with a Sol–Gel Method for Bone Implantation Kozik, Vladimir V.; Borilo, Lyudmila P.; Lyutova, Ekaterina S. ACS Omega, Vol. 5, Issue 42 https://doi.org/10.1021/acsomega.0c03335	journal	October 2020
The sol-gel process Hench, Larry L.; West, Jon K. Chemical Reviews, Vol. 90, Issue 1 https://doi.org/10.1021/cr00099a003	journal	January 1990
Synthesis and Characterization of High-Surface-Area Silica–Titania Monoliths Budnyk, Andriy; Damin, Alessandro; Bordiga, Silvia The Journal of Physical Chemistry C, Vol. 116, Issue 18 https://doi.org/10.1021/jp3012798	journal	May 2012
Toward Smart Implant Synthesis: Bonding Bioceramics of Different Resorbability to Match Bone Growth Rates Comesaña, Rafael; Lusquiños, Fernando; del Val, Jesús Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep10677	journal	June 2015
Bioactive functional materials: a perspective on phosphate-based glasses Abou Neel, Ensanya A.; Pickup, David M.; Valappil, Sabeel P. J. Mater. Chem., Vol. 19, Issue 6 https://doi.org/10.1039/B810675D	journal	January 2009
The evolution of ‘sol–gel’ chemistry as a technique for materials synthesis Danks, A. E.; Hall, S. R.; Schnepp, Z. Materials Horizons, Vol. 3, Issue 2 https://doi.org/10.1039/C5MH00260E	journal	January 2016
Non-aqueous template-assisted synthesis of mesoporous nanocrystalline silicon orthophosphate Styskalik, Ales; Skoda, David; Moravec, Zdenek RSC Advances, Vol. 5, Issue 90 https://doi.org/10.1039/C5RA10982E	journal	January 2015
Recent advances and future perspectives of sol–gel derived porous bioactive glasses: a review Deshmukh, Kalim; Kovářík, Tomáš; Křenek, Tomáš RSC Advances, Vol. 10, Issue 56 https://doi.org/10.1039/D0RA04287K	journal	January 2020
Phosphate based glasses for biomedical applications Knowles, Jonathan C. Journal of Materials Chemistry, Vol. 13, Issue 10 https://doi.org/10.1039/b307119g	journal	January 2003
Nanostructure evolution and calcium distribution in sol–gel derived bioactive glass Lin, Sen; Ionescu, Claudia; Pike, Kevin J. Journal of Materials Chemistry, Vol. 19, Issue 9 https://doi.org/10.1039/b814292k	journal	January 2009
Softening bioactive glass for bone regeneration: sol–gel hybrid materials Valliant, Esther M.; Jones, Julian R. Soft Matter, Vol. 7, Issue 11 https://doi.org/10.1039/c0sm01348j	journal	January 2011
Particle size distributions from small-angle scattering using global scattering functions Beaucage, G.; Kammler, H. K.; Pratsinis, S. E. Journal of Applied Crystallography, Vol. 37, Issue 4 https://doi.org/10.1107/S0021889804008969	journal	July 2004
Irena : tool suite for modeling and analysis of small-angle scattering Ilavsky, Jan; Jemian, Peter R. Journal of Applied Crystallography, Vol. 42, Issue 2 https://doi.org/10.1107/S0021889809002222	journal	February 2009
Approximations Leading to a Unified Exponential/Power-Law Approach to Small-Angle Scattering Beaucage, G. Journal of Applied Crystallography, Vol. 28, Issue 6 https://doi.org/10.1107/S0021889895005292	journal	December 1995
Development of combined microstructure and structure characterization facility for in situ and operando studies at the Advanced Photon Source Ilavsky, Jan; Zhang, Fan; Andrews, Ross N. Journal of Applied Crystallography, Vol. 51, Issue 3 https://doi.org/10.1107/S160057671800643X	journal	June 2018
Bioactive sol‐gel glasses: Processing, properties, and applications Baino, Francesco; Fiume, Elisa; Miola, Marta International Journal of Applied Ceramic Technology, Vol. 15, Issue 4 https://doi.org/10.1111/ijac.12873	journal	February 2018
Characterization, in vitro bioactivity and biological studies of sol‐gel‐derived TiO₂ substituted 58S bioactive glass Moghanian, Amirhossein; Nasiripour, Saba; Koohfar, Atiyyeh International Journal of Applied Ceramic Technology, Vol. 18, Issue 5 https://doi.org/10.1111/ijac.13782	journal	May 2021
Bioactive calcium phosphate–based glasses and ceramics and their biomedical applications: A review Islam, Md Towhidul; Felfel, Reda M.; Abou Neel, Ensanya A. Journal of Tissue Engineering, Vol. 8 https://doi.org/10.1177/2041731417719170	journal	January 2017
Bioactive glass scaffolds for bone regeneration and their hierarchical characterisation Jones, J. R.; Lin, S.; Yue, S. Proceedings of the Institution of Mechanical Engineers, Part H: Journal of Engineering in Medicine, Vol. 224, Issue 12 https://doi.org/10.1243/09544119JEIM836	journal	November 2010
Sol-gel as methodology to obtain bioactive materials Ribeiro, Thiago J.; Lima, Omar J. De; Faria, Emerson H. Anais da Academia Brasileira de Ciências, Vol. 86, Issue 1 https://doi.org/10.1590/0001-37652014106012	journal	March 2014
Properties and Applications of Metal Phosphates and Pyrophosphates as Proton Conductors Colodrero, Rosario M. P.; Olivera-Pastor, Pascual; Cabeza, Aurelio Materials, Vol. 15, Issue 4 https://doi.org/10.3390/ma15041292	journal	February 2022
Pore Structure and Fractal Characteristics of Different Shale Lithofacies in the Dalong Formation in the Western Area of the Lower Yangtze Platform Xu, Longfei; Zhang, Jinchuan; Ding, Jianghui Minerals, Vol. 10, Issue 1 https://doi.org/10.3390/min10010072	journal	January 2020
Treatment of Wastewaters with Zirconium Phosphate Based Materials: A Review on Efficient Systems for the Removal of Heavy Metal and Dye Water Pollutants Pica, Monica Molecules, Vol. 26, Issue 8 https://doi.org/10.3390/molecules26082392	journal	April 2021
Strontium Substituted β-Tricalcium Phosphate Ceramics: Physiochemical Properties and Cytocompatibility Fadeeva, Inna V.; Deyneko, Dina V.; Forysenkova, Anna A. Molecules, Vol. 27, Issue 18 https://doi.org/10.3390/molecules27186085	journal	September 2022

Similar Records

Optimization of TiO{sub 2} photoelectrode with titanium isopropoxide for flexible dye sensitized solar cells

Journal Article · 2016 · AIP Conference Proceedings · OSTI ID:22606696

Retnaningsih, Lilis; Muliani, Lia; Hidayat, Jojo

The role of TiO{sub 2} in the B{sub 2}O{sub 3}-Na{sub 2}O-PbO-Al{sub 2}O{sub 3} glass system

Journal Article · 2011 · Journal of Solid State Chemistry · OSTI ID:21580077

Sousa, N C.A. de; Araujo, M.T. de; Jacinto, C; +4 more

Raman scattering and XAFS study of optically nonlinear glasses of the TiO{sub 2}-NaPO{sub 3}-Na{sub 2}B{sub 4}O{sub 7} system

Journal Article · 1995 · Journal of Solid State Chemistry · OSTI ID:430267

Cardinal, T; Fargin, E; Le Flem, G

Related Subjects

36 MATERIALS SCIENCE

Title: Sol-gel derived silicate-phosphate glass SiO2–P2O5–CaO–TiO2: The effect of titanium isopropoxide on porosity and thermomechanical stability

Citation Formats

References (59)

Similar Records

Related Subjects

Title: Sol-gel derived silicate-phosphate glass SiO₂–P₂O₅–CaO–TiO₂: The effect of titanium isopropoxide on porosity and thermomechanical stability