Calcium silicate/calcium aluminate composite biocement for bone restorative application: Synthesis,characterisation and in vitro biocompatibility

Abstract

Pure β-dicalcium silicate and monocalcium aluminate powder were prepared by Pechini method. A series of calcium silicate/calcium aluminate cements (CSC/CAC) were prepared. The setting time, crystalline phases, microstructures, compressive strength, cells attachment and silicon release of the cements were investigated. The results indicate that the setting time of CSC/CAC was shorter than that of either CSC or CAC. The hydration products in CSC/CAC composite are gehlenite (Ca₂Al₂SiO₇·8H₂O), calcium aluminate hydrate (Ca₃Al₂O₆× H₂O), and katoite (Ca₂Al₂O₆·6H₂O). Platelike crystals were found in the microstructure. The liquid to powder ratio has a significant effect on the porosity and the strength of CSC/CAC. The MC3T3 cells attached well to the surfaces of CSC/CAC. However, the cells proliferation on the surface of 7S3A was better than that of 3S7A due to its higher silicon release. In general, CSC/CAC exhibits good biocompatibility and relative high strength, and may be suitable for some non-load bearing bone restorative applications.

Keywords

Hydration Mechanical properties Calcium silicate cement Calcium aluminate cement Composite Inorganic bone cement

Get full access to this article

View all access options for this article.

References

Ishikawa

and Asaoka

: ‘Estimation of ideal mechanical strength and critical porosity of calcium phosphate cement’, J. Biomed. Mater. Res., 1995, 29, (12), 1537–1543. doi: 10.1002/jbm.820291210

Piecuch

J. F.

: ‘Extraskeletal of a porous hydroxyapatite ceramic’, J. Dent. Res., 1982, 61, (12), 1458–1460. doi: 10.1177/00220345820610121801

Kitsugi

, Yamamuro

, Takeuchi

and Ono

: ‘Bonding behavior of three types of hydroxyapatite with different sintering temperatures implanted in bone’, Clin. Orthop. Relat. Res., 1988, 234, 280–290.

, Wei

, Guo

, Chen

F. P.

, Hong

and Liu

C. S.

: ‘Self-setting bioactive calcium–magnesium phosphate cement with high strength and degradability for bone regeneration’, Acta Biomater., 2008, 4, (6), 1873–1884. doi: 10.1016/j.actbio.2008.06.020

Ratner

Buddy D.

, Hoffman

Allan S.

, Schoen

Frederick J.

and Lemons

J. E.

: ‘Biomaterials science: an introduction to materials in medicine’, 3rd edn; 2013, Oxford, Academic Press.

Lee

K.-Y.

, Park

, Kim

H.-M.

, Lim

Y.-J.

, Chun

H.-J.

, Kim

and Moon

S.-H.

: ‘Ceramic bioactivity: progresses, challenges and perspectives’, Biomed Mater., 2006, 1, (2), R31. doi: 10.1088/1748-6041/1/2/R01

, Shi

, Zhu

, Shen

, Li

, Liang

and Gao

: ‘A template route to the preparation of mesoporous amorphous calcium silicate with high in vitro bone-forming bioactivity’, J. Biomed. Mater. Res. B, 2007, 83B, (2), 431–439. doi: 10.1002/jbm.b.30813

Sprio

, Tampieri

, Celotti

and Landi

: ‘Development of hydroxyapatite/calcium silicate composites addressed to the design of load-bearing bone scaffolds’, J. Mech. Behav. Biomed. Mater., 2009, 2, (2), 147–155. doi: 10.1016/j.jmbbm.2008.05.006

Taddei

, Tinti

, Gandolfi

M. G.

, Rossi

P. L.

and Prati

: ‘Ageing of calcium silicate cements for endodontic use in simulated body fluids: a micro-Raman study’, J. Raman Spectrosc., 2009, 40, (12), 1858–1866. doi: 10.1002/jrs.2333

10.

, Zhu

Y. J.

, Chen

, Zhao

X. Y.

, Zhao

and Qi

: ‘Amorphous calcium silicate hydrate/block copolymer hybrid nanoparticles: synthesis and application as drug carriers’, Dalton Trans., 2013, 42, (19), 7032–7040. doi: 10.1039/c3dt50143d

11.

Hughes

, Yanni

, Jamshidi

and Grover

: ‘Inorganic cements for biomedical application: calcium phosphate, calcium sulphate and calcium silicate’, Adv. Appl. Ceram., 2015, 114, (2), 65–76. doi: 10.1179/1743676114Y.0000000219

12.

Tan

, Yong

, Qing

, Birdi

and Grover

L. M.

: ‘Synthesis of pure dicalcium silicate powder by the Pechini method and characterization of hydrated cement’, Mater. Sci. Forum, 2014, Trans Tech Publ, 387–394. doi: 10.4028/www.scientific.net/MSF.787.387

13.

Ding

S. J.

, Shie

M. Y.

and Wang

C. Y.

: ‘Novel fast-setting calcium silicate bone cements with high bioactivity and enhanced osteogenesis in vitro’, J. Mater. Chem., 2009, 19, (8), 1183–1190. doi: 10.1039/b819033j

14.

Correa

, Almirall

, Garcia-Carrodeguas

, Alberto Dos Santos

, De Aza

A. H.

, Parra

and Angel Delgado

: ‘Beta-dicalcium silicate-based cement: synthesis, characterization and in vitro bioactivity and biocompatibility studies’, J. Biomed. Mater. Res. A, 2014, 102, (10), 3693–3703. doi: 10.1002/jbm.a.35041

15.

Nettleship

, Shull

J. L.

and Kriven

W. M.

: ‘Chemical preparation and phase-stability of Ca₂SiO₄ and Sr₂SiO₄ powders’, J. Eur. Ceram. Soc., 1993, 11, (4), 291–298. doi: 10.1016/0955-2219(93)90028-P

16.

Tan

, Liu

, Zhang

, Hofmann

and Grover

: ‘Comparing three methods for the synthesis of pure β-dicalcium silicate’, 4rd International Conference on Bioinformatics and Biomedical Engineering, iCBBE 2010, 2010.

17.

Odler

: ‘Special inorganic cements’; 2000, Boca Raton, FL, CRC Press.

18.

Van Dijken

J. W.

and Sunnegårdh-Grönberg

: ‘A three year follow-up of posterior doxadent restorations’, Swiss dent., 2005, 29, (2), 45–51.

19.

Franz

, Konradsson

, Konig

, Van Dijken

J. W. V.

and Schedle

: ‘Cytotoxicity of a calcium aluminate cement in comparison with other dental cements and resin-based materials’, Acta Odontol. Scand., 2006, 64, (1), 1–8. doi: 10.1080/00016350500279568

20.

Loof

, Engqvist

, Ahnfelt

N. O.

, Lindqvist

and Hermansson

: ‘Mechanical properties of a permanent dental restorative material based on calcium aluminate’, J. Mater. Sci.-Mater. Med., 2003, 14, (12), 1033–1037. doi: 10.1023/B:JMSM.0000003999.52349.0d

21.

Tan

, Liu

, Zhang

, Huang

and Grover

L. M.

: ‘hydroxyapatite formation on surface of calcium aluminate cements’, Adv. Appl. Ceram., 2011, 110, (8), 464–468. doi: 10.1179/1743676111Y.0000000033

22.

Anon : ‘Silica by Colorimetry’, Method#:370.1, 1978, www.ezkem.com/resources/articles/EPA_Methods/370_1.pdf .

23.

S. H.

, Choi

S. Y.

, Lee

Y. K.

, Kim

K. N.

and Choi

S. H.

: ‘Effects of lithium fluoride and maleic acid on the bioactivity of calcium aluminate cement: formation of hydroxyapatite in simulated body fluid’, J. Biomed. Mater. Res. A, 2003, 67A, (1), 104–111. doi: 10.1002/jbm.a.10036

24.

S. H.

, Choi

S. Y.

, Lee

Y. K.

and Kim

K. N.

: ‘Preparation of calcium aluminate cement for hard tissue repair: effects of lithium fluoride and maleic acid on setting behavior, compressive strength, and biocompatibility’, J. Biomed. Mater. Res., 2002, 62, (4), 593–599. doi: 10.1002/jbm.10347

25.

Damidot

and Glasser

F. P.

: ‘Investigation of the CaO–Al₂O₃–SiO₂–H₂O system at 25°C by thermodynamic calculations’, Cement Concrete Res., 1995, 25, (1), 22–28. doi: 10.1016/0008-8846(94)00108-B

26.

Skibsted

, Henderson

and Jakobsen

H. J.

: ‘Characterization of calcium aluminate phases in cements by aluminum-27 MAS NMR spectroscopy’, Inorg. Chem., 1993, 32, (6), 1013–1027. doi: 10.1021/ic00058a043

27.

Matusinovic

, Sipusic

and Vrbos

: ‘Porosity-strength relation in calcium aluminate cement pastes’, Cement Concrete Res., 2003, 33, (11), 1801–1806. doi: 10.1016/S0008-8846(03)00201-1

28.

Gou

, Chang

, Zhai

and Wang

: ‘Study on the self-setting property and the in vitro bioactivity of beta-Ca₂SiO₄’, J. Biomed. Mater. Res. B, 2005, 73B, (2), 244–251. doi: 10.1002/jbm.b.30203

29.

Villacampa

A. I.

and Garcı´a-Ruiz:

J. M.

‘Synthesis of a new hydroxyapatite-silica composite material’, J. Cryst. Growth, 2000, 211, (1), 111–115. doi: 10.1016/S0022-0248(99)00793-9

30.

Sousa

, Souza

and Sousa

: ‘Mesoporous silica/apatite nanocomposite: special synthesis route to control local drug delivery’, Acta Biomater., 2008, 4, (3), 671–679. doi: 10.1016/j.actbio.2007.11.003

31.

Saenz

, Montero

and Castano

: ‘Preparation of silica–hydroxyapatite nanometric composites’, Phys. Status Solidi B, 2002, 230, (2), 347–350. doi: 10.1002/1521-3951(200204)230:2<347::AID-PSSB347>3.0.CO;2-I

32.

Ning

, Mehta

and El-Ghannam

: ‘Effects of silica on the bioactivity of calcium phosphate composites in vitro’, J. Mater. Sci.-Mater. Med., 2005, 16, (4), 355–360. doi: 10.1007/s10856-005-0635-8