Sains Malaysiana 51(3)(2022): 883-894

http://doi.org/10.17576/jsm-2022-5103-22

Fabrication of Magnesium-Carbonate Apatite by Conventional Sintering and Spark Plasma Sintering for Orthopedic Implant Applications

(Fabrikasi Magnesium-Karbonat Apatit oleh Pensinteran Konvensional dan Pensinteran Percikan Plasma untuk Aplikasi Implan Ortopedik)

IWAN SETYADI^1,2, TOTO SUDIRO³, BAMBANG HERMANTO³, PRIMA RIZKY OKTARI⁴, ACHMAD FAUZI KAMAL⁴, AHMAD JABIR RAHYUSSALIM⁴, BAMBANG SUHARNO⁵ & SUGENG SUPRIADI⁶

¹Department of Metallurgical and Materials Engineering, Faculty of Engineering, Universitas Indonesia, Depok, I 16424, Indonesia

²Center for Material Technology, Agency for the Assessment and Application of Technology (BPPT)-Indonesia  

³Research Center for Physics (P2Fisika), Indonesian Institute of Sciences (LIPI), Indonesia  

⁴Department Orthopedic and Traumatology, Faculty of Medicine, Universitas Indonesia, Indonesia  

⁵Department of Metallurgical and Materials Engineering, Faculty of Engineering, Universitas Indonesia, Indonesia  

⁶Department of Mechanical Engineering, Universitas Indonesia, Indonesia

Received: 27 April 2021/Accepted: 15 August 2021

ABSTRACT

Magnesium-Carbonate Apatite (Mg-xCA) is one of the potential magnesium composites to be developed as an alternative biodegradable implant material. Several attempts were made to optimize its characteristics. In this study, Mg-xCA (x = 0, 5, 10, and 15% wt) was prepared by powder metallurgy through warm compaction (WC) and further densified by 2 sintering process methods, namely conventional sintering (CS) and spark plasma sintering (SPS). The characterization included density test, XRD test, microstructure test (OM and SEM-EDS-Mapping), microhardness test, and electrochemical test. The SPS process improves the characteristics of Mg-xCA better than the CS process. The SPS process can increase the relative density by about 0.7-2.4%, increase the hardness by about 2-13%, and reduce the corrosion rate by about 32-49% compared to the initial condition before sintering (WC). The SPS structure has a lower oxygen elemental content than the CS structure. The sintered process with SPS is considered effective for the fabrication of Mg-xCA powder-based composites compared to the CS process.

Keywords: Characterization; conventional sintering; magnesium-carbonate apatite; spark plasma sintering

ABSTRAK

Magnesium-Karbonat Apatit (Mg-xCA) adalah salah satu komposit magnesium yang berpotensi untuk dikembangkan sebagai bahan implan biodegradasi alternatif. Beberapa usaha dilakukan untuk mengoptimumkan ciri-cirinya. Dalam kajian ini, Mg-xCA (x = 0, 5, 10, dan 15% wt) disiapkan oleh metalurgi serbuk melalui pemadatan suam(WC) dan selanjutnya diperkecilkan dengan 2 kaedah proses pensinteran, iaitu pensinteran konvensional(CS) dan percikan plasma pensinteran(SPS). Pencirian tersebut merangkumi ujian kepadatan, ujianXRD, ujian struktur mikro (OM dan SEM-EDS-Pemetaan), ujian kekerasan mikro dan ujian elektrokimia. Proses SPS meningkatkan ciri Mg-xCA lebih baik daripada proses CS. Proses SPS dapat meningkatkan ketumpatan relatif sekitar 0.7-2.4%, meningkatkan kekerasan sekitar 2-13% dan mengurangkan kadar kakisan sekitar 32-49% dibandingkan dengan keadaan awal sebelum pensinteran(WC). Struktur SPS mempunyai kandungan unsur oksigen yang lebih rendah daripada strukturCS. Proses pensinteran denganSPS dianggap berkesan untuk pembuatan komposit berasaskan serbukMg-xCA berbanding dengan proses CS.

Kata kunci: Magnesium-karbonat apatit; pencirian; pensinteran konvensional; pensinteran plasma percikan

REFERENCES

Ahmad Jabir Rahyussalim, Aldo Fransiskus Marsetio, Achmad Fauzi Kamal, Sugeng Supriadi, Iwan Setyadi, Pancar Muhammad Pribadi, Wildan Mubarok & Tri Kurniawati. 2021. Synthesis, structural characterization, degradation rate, and biocompatibility of magnesium-carbonate apatite (Mg-Co3Ap) composite and its potential as biodegradable orthopaedic implant base material. Journal of Nanomaterials 2021: 6615614. https://doi.org/10.1155/2021/6615614.

Ahmad Jabir Rahyussalim, Sugeng Supriadi, Achmad Fauzi Kamal, Aldo Fransiskus Marsetio & Pancar Muhammad Pribadi. 2019. Magnesium-carbonate apatite metal composite: Potential biodegradable material for orthopaedic implant. In AIP Conference Proceedings 2092: 20021. AIP Publishing LLC. https://doi.org/10.1063/1.5096689.

Annur, D. 2017. Powder metallurgy preparation of Mg-Ca Alloy for biodegradable implant application to. Journal of Physics: IOP Conference Series 817. https://doi.org/10.1088/1742-6596/817/1/012062.

Ayukawa Yasunori, Yumiko Suzuki, Kanji Tsuru, Kiyoshi Koyano & Kunio Ishikawa. 2015. Histological comparison in rats between carbonate apatite fabricated from gypsum and sintered hydroxyapatite on bone remodeling. BioMed Research International https://doi.org/10.1155/2015/579541.

ASTM E384-17. 2017. Standard Test Method for Microindentation Hardness of Materials.

ASTM. G102-89. 2015. Standard Practice for Calculation of Corrosion Rates and Related Information from Electrochemical Measurements.

ASTM. G5-94. 2014. Standard Reference Test Method for Making Potentiodynamic Anodic Polarization Measurements.

Atmaja Surbakti, Maximillian Ch. Oley & Eko Prasetyo. 2017. Perbandingan antara penggunaan karbonat apatit dan hidroksi apatit pada proses penutupan defek kalvaria dengan menggunakan plasma kaya trombosit. Jurnal Biomedik (Jbm) 9(2): 107-114. https://doi.org/10.35790/jbm.9.2.2017.16359.

Center for Material Technology (BPPT). 2017. Technical Note GL3/Alkes.

Del Campo, R., Savoini, B., Muñoz, A., Monge, M.A. & Pareja, R. 2017. Processing and mechanical characteristics of magnesium-hydroxyapatite metal matrix biocomposites. Journal of the Mechanical Behavior of Biomedical Materials 69: 135-143. https://doi.org/10.1016/j.jmbbm.2016.12.023.

Del Campo, R., Savoini, B., Muñoz, A., Monge, M.A. & Garcés, G. 2014. Mechanical properties and corrosion behavior of Mg-HAP composites. Journal of the Mechanical Behavior of Biomedical Materials 39: 238-246. https://doi.org/10.1016/j.jmbbm.2014.07.014.

Doi, Y., Koda, T., Adachi, M., Wakamatsu, N., Goto, T., Kamemizu, H., Moriwaki, Y. & Suwa, Y. 1995. Pyrolysis-gas chromatography of carbonate apatites used for sintering. Journal of Biomedical Materials Research 29(11): 1451-1457. https://doi.org/10.1002/jbm.820291117.

Godavitarne, C., Robertson, A., Peters, J. & Rogers, B. 2017. Biodegradable materials. Orthopaedics and Trauma 31(5): 316-320. https://doi.org/10.1016/j.mporth.2017.07.011.

Gu, X-N. & Zheng, Y-F. 2010. A review on magnesium alloys as biodegradable materials. Frontiers of Materials Science in China 4(2): 111-115. https://doi.org/10.1007/s11706-010-0024-1.

Gu, X., Zhou, W., Zheng, Y., Dong, L., Xi, Y. & Chai, D. 2010. Microstructure, mechanical property, bio-corrosion and cytotoxicity evaluations of Mg/HA composites. Materials Science and Engineering: C 30(6): 827-832. https://doi.org/10.1016/j.msec.2010.03.016.

Haghshenas, M. 2017. Mechanical characteristics of biodegradable magnesium matrix composites: A review. Journal of Magnesium and Alloys 5(2): 189-201. https://doi.org/10.1016/j.jma.2017.05.001.

Hirokazu Nagai, Masako Kobayashi-Fujioka, Kenji Fujisawa, Go Ohe, Natsumi Takamaru, Kanae Hara, Daisuke Uchida, Tetsuya Tamatani, Kunio Ishikawa & Youji Miyamoto. 2015. Effects of low crystalline carbonate apatite on proliferation and osteoblastic differentiation of human bone marrow cells. Journal of Materials Science: Materials in Medicine 26(2): 1-8. https://doi.org/10.1007/s10856-015-5431-5.

Ishikawa, K. 2019. Carbonate apatite bone replacement: Learn from the bone. Journal of the Ceramic Society of Japan 127(9): 595-601. https://doi.org/10.2109/jcersj2.19042.

Iwan Setyadi, Aldo Fransiskus Marsetio, Achmad Fauzi Kamal, Rahyussalim, Sugeng Supriadi & Bambang Suharno. 2020a. Microstructure and microhardness of carbonate apatite particle-reinforced Mg composite consolidated by warm compaction for biodegradable implant application. Materials Research Express 7(5). https://doi.org/10.1088/2053-1591/ab7d70.

Iwan Setyadi, Pancar Muhammad Pribadi, Aldo Fransiskus Marsetio, Achmad Fauzi Kamal, Rahyusalim, Bambang Suharno & Sugeng Supriadi. 2020b. Characteristics investigation of the initial development of miniplate made from composite of magnesium/carbonate apatite fabricated by powder metallurgy method for biodegradable implant applications. In Key Engineering Materials 833 KEM: 194-198. Trans Tech Publications Ltd. https://doi.org/10.4028/www.scientific.net/KEM.833.194.

Jaiswal, S., Manoj Kumar, R., Gupta, P., Kumaraswamy, M., Roy, P. & Lahiri, D. 2018. Mechanical, corrosion and biocompatibility behaviour of Mg-3Zn-HA biodegradable composites for orthopaedic fixture accessories. Journal of the Mechanical Behavior of Biomedical Materials 78: 442-454. https://doi.org/10.1016/j.jmbbm.2017.11.030.

Kingston Technical Software. n.d. Corrosion Rate Conversion. https://www.corrosion-doctors.org/Principles/Conversion.htm.

Kokubo, T., Kushitani, H., Sakka, S., Kitsugi, T. & Yamamuro, T. 1990. Solutions able to reproduce in vivo surface‐structure changes in bioactive glass‐ceramic A‐W3. Journal of Biomedical Materials Research 24(6): 721-734. https://doi.org/10.1002/jbm.820240607.

Kuśnierczyk, K. & Basista, M. 2017. Recent advances in research on magnesium alloys and magnesium–calcium phosphate composites as biodegradable implant materials. Journal of Biomaterials Applications 31(6): 878-900. https://doi.org/10.1177/0885328216657271.

Landi, E., Celotti, G., Logroscino, G. & Tampieri, A. 2003. Carbonated hydroxyapatite as bone substitute. Journal of the European Ceramic Society 23(15): 2931-2937. https://doi.org/10.1016/S0955-2219(03)00304-2.

Linhart, W., Peters, F., Lehmann, W., Schwarz, K., Schilling, A.F., Amling, M., Rueger, J.M. & Epple, M. 2000. Biologically and chemically optimized composites of carbonated apatite and polyglycolide as bone substitution materials. J. Biomed. Mater. Res. 54(2): 162-171.

Liu, R., Wang, W., Chen, H., Lu, Z., Zhao, W. & Zhang, T. 2019. Densification of pure magnesium by spark plasma sintering-discussion of sintering mechanism. Advanced Powder Technology 30(11): 2649-2658. https://doi.org/10.1016/j.apt.2019.08.012.

Madupalli, H., Pavan, B. & Tecklenburg, M.M.J. 2017. Carbonate substitution in the mineral component of bone: Discriminating the structural changes, simultaneously imposed by carbonate in A and B sites of apatite. Journal of Solid State Chemistry 255: 27-35. https://doi.org/10.1016/j.jssc.2017.07.025.

Masayuki Kanazawa, Kanji Tsuru, Naoyuki Fukuda, Yuta Sakemi, Yasuharu Nakashima & Kunio Ishikawa. 2017. Evaluation of carbonate apatite blocks fabricated from dicalcium phosphate dihydrate blocks for reconstruction of rabbit femoral and tibial defects. Journal of Materials Science: Materials in Medicine 28(6): 85. https://doi.org/10.1007/s10856-017-5896-5.

Mohammad Khodaei, Farahnaz Nejatidanesh, Mohammad Javad Shirani, Srinivasan Iyengar, Hossein Sina & Omid Savabi. 2020. Magnesium/nano-hydroxyapatite composite for bone reconstruction: The effect of processing method. Journal of Bionic Engineering 17(1): 92-99. https://doi.org/10.1007/s42235-020-0007-6.

Mahmoud Abbas Ibraheem, Abd El Aziz El Sayed Fouda, Mohamed Talaat Rashad & Fawzy Nagy Sabbahy. 2012. Sweet corrosion inhibition on API 5L-B pipeline steel. International Scholarly Research Notices 2012: 892385. https://doi.org/10.5402/2012/892385.

NN n.d. Spark Plasma Sintering. http://www.subtech.com/dokuwiki/doku.php? id = spark_plasma_sintering. Accessed on December 3, 2019.

Radha, R. & Sreekanth. D. 2017. Insight of magnesium alloys and composites for orthopedic implant applications - A review. Journal of Magnesium and Alloys 5(3): 286-312. https://doi.org/10.1016/j.jma.2017.08.003.

Siska Wiwanto, Lilies Dwi Sulistyani, Fourier Dzar Eljabbar Latief, Sugeng Supriadi, Bambang Pontjo Priosoeryanto & Benny Syariefsyah Latief. 2018. The experiment of magnesium ECAP miniplate as alternative biodegradable material (on male white New Zealand rabbits). In AIP Conference Proceedings, 1933: 20013. AIP Publishing LLC. https://doi.org/10.1063/1.5023947.

Sunil, B.R., Ganapathy, C., Sampath Kumar, T.S. & Chakkingal, U. 2014. Processing and mechanical behavior of lamellar structured degradable magnesium–Hydroxyapatite implants. Journal of the Mechanical Behavior of Biomedical Materials 40: 178-189. https://doi.org/10.1016/j.jmbbm.2014.08.016.

Supriadi, S., Kristianto, H., Whulanza, Y., Saragih, A.S., Dhelika, R., Latief, B.S. & Taufiq, T. 2018. Fabrication of magnesium ECAP based maxillary miniplate-typed implant through the method of micro forming. IOP Conference Series: Materials Science and Engineering 432: 012037. https://doi.org/10.1088/1757-899X/432/1/012037.

Witte, F., Feyerabend, F., Maier, P., Fischer, J., Störmer, M., Blawert, C., Dietzel, W. & Hort, N. 2007. Biodegradable magnesium-Hydroxyapatite metal matrix composites. Biomaterials 28(13): 2163-2174. https://doi.org/10.1016/j.biomaterials.2006.12.027.

Xiong, G., Nie, Y., Ji, D., Li, J., Li, C., Li, W., Zhu, Y., Luo, H. & Wan, Y. 2016. Characterization of biomedical hydroxyapatite/magnesium composites prepared by powder metallurgy assisted with microwave sintering. Current Applied Physics 16(8): 830-836. https://doi.org/10.1016/j.cap.2016.05.004.

Youness, R.A., Taha, M.A. & Ibrahim, M.A. 2017. Effect of sintering temperatures on the in vitro bioactivity, molecular structure and mechanical properties of titanium/carbonated hydroxyapatite nanobiocomposites. Journal of Molecular Structure 1150: 188-195. https://doi.org/10.1016/j.molstruc.2017.08.070.

Yunita Sari & Siska Titik Dwiyati. 2015. Korosi H2S dan CO2 pada peralatan statik di industri minyak dan gas. Jurnal Konversi Energi dan Manufaktur UNJ 2(1): 18-22.

Zheng, Y.F., Gu, X.N. & Witte, F. 2014. Biodegradable metals. Materials Science and Engineering: R: Reports 77: 1-34. https://doi.org/10.1016/j.mser.2014.01.001.

^*Corresponding author; email: i1setyadi2810@gmail.com