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Coating of stainless steel 304 surface with apatite compound using the electrophoretic deposition method
Conference Paper in AIP Conference Proceedings · November 2022
DOI: 10.1063/5.0103222
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AIP Conference Proceedings 2542, 050016 (2022); https://doi.org/10.1063/5.0103222 2542, 050016
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Coating of stainless steel 304 surface with apatite compound using the electrophoretic deposition method
Cite as: AIP Conference Proceedings 2542, 050016 (2022); https://doi.org/10.1063/5.0103222 Published Online: 10 November 2022
M. Sari, Ishak Pawarangan, D. U. Khasanah, et al.
Coating of Stainless Steel 304 Surface with Apatite Compound Using the Electrophoretic Deposition Method
M. Sari
1, Ishak Pawarangan
1, 2, a), D. U. Khasanah
1, F. Y. Syafaat
1, V. J. Mawuntu
1, Y. Rizkayanti
1, A. Kusumaatmadja
1, Y. Yusuf
11Department of Physics, Universitas Gadjah Mada, Sekip Utara BLS 21, Yogyakarta 55281, Indonesia
2Faculty of Engineering, Universitas Kristen Indonesia Toraja, 91853, Indonesia
a)Corresponding author: [email protected]
Abstract. Stainless steel 304 is a metal used to replace damaged bones. However, this metal has a low level of biocompatibility in the body. To solve this problem, the metals are coated with a biocompatible material before implantation. The material used to coat the stainless steel is an apatite compound derived from eggshell because the composition of minor minerals of eggshell was CaCO3 94%, MgCO3 1%, CaPO4 1%, and organic material 4%. The method used in this research is the electrophoretic deposition method. This research aims to study the effect of apatite compounds that are coating on stainless steel 304 surfaces. Based on the experimental results, the suspension process carried out pH controls that resulted in pH 11.15, 1.42, 3.86, and 4.55. Increasing and decreasing pH can occur because the compound of HNO3 and NH4OH was strong acid and base. Researchers were not very careful in measuring the volume of HNO3 and NH4OH when it was inserted into the apatite compound suspension. The pH of the suspension affected the potential value (ζ), which indicated the stability of the particle resistance and determined the direction and speed of migration during the EPD process. Using the apatite compound concentration affected the mass of apatite compounds deposited on the stainless steel 304. Based on the experimental results, apatite compounds can attach to the stainless steel 304 surface.
INTRODUCTION
Osteoporosis is one of the leading causes of bone damage. Although osteoporosis is more related to the elderly, bone loss can affect anyone, even the young people. A recent study by the International Osteoporosis Foundation (IOF) showed that one in four Indonesian women between the ages of 50 and 80 are at risk of osteoporosis. Their risk is four times that of Indonesian men. A study conducted by the Indonesian Osteoporosis Association in 2007 reported that the proportion of osteoporosis patients over 50 years old was 32.3% for women and 28.8% for men [1].
Generally, the treatment of bone injury involves the use of heavy metals to replace the damaged bone. However, this poses a problem because the level of biocompatibility of the metal in the body is low, which can cause disease or bruising of the tissue surrounding the metal. To solve this problem, the metal is coated with a biocompatible material before implantation. Previously, these coatings were made from materials already present in the body: components of bone tissue, such as apatite compounds. However, an artificial bone compound similar to the original bone composition is now available: hydroxyapatite [2].
Hydroxyapatite, Ca10(PO4)6(OH)2 or simpler HA, is an essential part of human bones and teeth [3]. It is commonly used in orthopedics, dentistry, and maxillofacial applications [4–6]. HA has a stable potassium phosphate crystal phase, hexagonal structure, lattice parameters a = 9.433Å, c = 6.875Å, and a variable Ca/P molar ratio of 1.67 [7–9].
The advantages of hydroxyapatite are porous, bioactive, non-corrosive, and wear-resistant. The weight of HA is 69%
of the importance of pure bone, and it is the most stable compound in body fluids and dry air, with a temperature as high as 1200 ℃ [10].
Chemically synthesized HA is called synthetic HA. Synthetic HA can be obtained by reacting to synthetic compounds and by responding with natural compounds. HA can be synthesized from high calcium materials, such as buffalo bones, fish bones, cuttlefish, eggshells, and mussel shells [2, 8].
The 4th International Conference on Science and Science Education (IConSSE 2021) AIP Conf. Proc. 2542, 050016-1–050016-6; https://doi.org/10.1063/5.0103222
Published by AIP Publishing. 978-0-7354-4259-7/$30.00
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Here, the eggshells from Indonesia are used as the natural compound for chemical synthesis. Based on the Central Bureau of Statistics (2009), eggshells are plentiful in Indonesia that is ± 86.000 tons or 10 % of egg production per year. Eggshells have not been utilized, so it has become waste, while eggshells are one source of CaCO3. The minor mineral composition in eggshells is CaCO3 94%, MgCO3 1%, CaPO4 1%, and organic material 4%. Especially, chicken eggshells have the highest Ca (70.84%). It compared to quail eggshells (55.46%) and duck eggshells (53.60%). Chicken eggshells powder contained 401 ± 7.2 gram or about Ca (39%) in the form of CaCO3 [11].
Although HA implants are biocompatible and bioactive, they have the disadvantages of tensile strength and toughness. This result can affect long-term complications such as pain, inflammation, and loose implants. One of the innovations is using HA as the surface coating (coated with hydroxyapatite) of metal implants [12].
Most metals used for hydroxyapatite coatings are usually made of 316L stainless steel (ASTM F138), cobalt alloys (ASTM F75 and F799), pure titanium, and Ti6A14V titanium alloys (ASTM F67 and F136) [13]. In this study, the apatite composite powder was coated with 304 stainless steel because it is non-toxic, strong, non-corrosive, and has low impurities.
Several techniques for coating hydroxyapatite on metal surfaces are dip coating, electrophoretic deposition (EPD), sol-gel coating, and plasma spraying. Apatite coating is an electrochemical method. The processes commonly used for the electrodeposition of apatite on metals and other bioceramics are electrodeposition and electrophoresis. One of the studies that have successfully coated stainless steel is the EPD method. In this case, stainless steel will be the target of fixation on the EPD electrode. EPD apatite coating technology is simple alternative technology with low processing cost and the ability to form layers with complex shapes [14].
EPD is an electrochemical method used as a technique for material coating processes. EPD includes the movement of electrical charges applied to the surface of the metallic coating under the influence of an electric field. The schematic diagram of moving particles is shown in Fig. 1. In the second stage, the particles of the apatite compound will deposit on the metal surface of the electrode and uniformly seal the metal surface in the form of a film. This layer results from the deposition of particles of apatite compound adhered to stainless steel [15]. The purpose of this study is The purpose of this study is evaluating the coating of apatite compounds on stainless steel 304 substrates by using EPD method under pH control.
FIGURE 1. Movement of the particle in a stable suspension. Particles with positive charges
will move toward the negative electrode [15].
METHOD Preparation
This process began by calculating the volume of HNO3 65% and H2O required for 3M based on the dilution principle. The same treatment was also done in NH4OH 25% 3M. As shown in Fig. 2, stainless steel 304 plates were cleaned with 500-grid and 1000-grid sandpaper paper, and it cleaned again using the distilled water. This was done to remove any dirt on the metal surface. The apatite compound was suspended with the addition of ethanol. The suspension of 0.025M was mixed with 0.452 grams of apatite compound and 25 ml of ethanol. Then, the mixture of the solution was stirred using a magnetic stirrer with a stirring speed of 200 rpm for 30 min until the apatite compound was dispersed in an ethanol solution. It can be shown by a cloudy suspension of particles. Furthermore, during the
agitation process, the apatite compound suspension was adjusted to pH 3 and pH 4 by added HNO3 3M. Then, Addition a little solution of NH4OH 3M was done to adjust the pH 10.
(a) (b) (c)
FIGURE 2. (a) Preparation of stainless steel 304, (b) suspension of apatite compound, and (c) control of pH.
Coating of Apatite Compound in Stainless Steel 304
Suspension of apatite compound is signed into beaker glass. As shown in Fig. 3, this solution was connected to both electrodes. One electrode was a stainless steel plate which was the target of apatite compound coated on its surface (negatively charged), and the other was a carbon electrode (positively charged). Two electrodes were connected to a power supply (60 V for one hour). In the electrophoretic deposition process, the power of the apatite compound dispersed in the solution will be driven by electrophoresis. The apatite compound that carried over would attach to different metal surfaces [15]. After the coating process was complete, the samples were calcined using a furnace at 100℃ for 30 min.
FIGURE 3. Coating of apatite compound in stainless steel 304 plate surface.
RESULT AND DISCUSSIONS
Coating of stainless steel 304 with apatite compound used the electrophoretic deposition method. In this experiment, pH controls were 3, 4, and 10. Based on experimental results, when NH4OH solution was added for the first time, the suspension pH increased dramatically to 11.15. Therefore, the researcher directly added HNO3 1 ml, so the suspension pH decreased dramatically to 1.42. Then, the researcher added a drop of NH4OH solution, so the pH
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increased to 3.86. They added another drop of NH4OH solution, the pH of apatite suspension became 4.55. Increasing and decreasing pH can occur because the compound of HNO3 and NH4OH was strong acid and base, so that addition can significantly affect the suspension of the apatite compound. Researchers were not very careful in measuring the volume of HNO3 and NH4OH when it was inserted into the apatite compound suspension.
The pH of the suspension affected the potential value (ζ), which indicated the stability of the particle resistance and determined the direction and speed of migration during the EPD process. Using the amount of apatite compound concentration affected the mass of apatite compounds deposited on the surface of stainless steel 304 [15].
The EPD mechanism consisted of two stages. In the first stages, the flow of electricity between two electrodes would make the stainless steel 304 as the cathode (-) and the carbon electrode as the anode (+). Apatite compound is made of an HA-containing solution, which tends to have a positive charge. Element Ca in the apatite compound is more likely to move because the Ca-weighted charge was greater than P. When the electrodes are introduced in the solution, Ca tended to move toward negative electrodes (cathodes), which we prepared Stainless steel 304 in this research. During the electrophoresis process, it was observed that tiny air bubbles were formed on the stainless steel 304 surface. It occurred because of a cathodic reaction that created H2 gas, as shown in Eq. 1. and Eq. 2.
2H!O + 2e"→ H!+ 2OH" (1) H!O + e"→!"H!+ OH" (2) The second stage of the EDP process was the deposition process, which leads apatite compound with a positive charge (+) to move toward stainless steel 304 as the negative electrode (cathode). Figure 4 shows the process of the apatite compound movement. Apatite particle which reached stainless steel 304 electrode then sticks on the plate surface. As it increases and piles up, forming a layer of apatite compound, it became more robust and complex.
FIGURE 4. EDP Process in coating Stainless Steel 304 with apatite compound.
After the electrophoretic process is done, the next stage is the deposition or attachment of apatite particles on the stainless steel 304 surface. The samples are calcined using a furnace at 100℃ for 30 min. Figure 5 shows the result of the calcination process, which can be seen that the apatite compound is firmly attached on the stainless steel 304 metal surface.
FIGURE 5. Final result: Apatite compound attached in stainless steel 304 plate surfaces.
This research shows that the coating layer of apatite compound formed from EPD was not distributed equally on the stainless steel 304 surface. The coating layer is formed very thick in the middle area but poorly attached to the side area of the plate. This inhomogeneous layer occurred because the side area of the plate was more likely to have a higher deposition process in a liquid environment than the middle area of the plate.
CONCLUSION
Apatite compound coatings were successfully deposited on stainless steel 304 substrates by EPD under pH controls suspension to study the effect of pH controls on apatite compound coating. The coating process consists of two stages:
electrophoretic of apatite compound and deposition of apatite compound on a stainless steel 304 metal surface. Based on the experimental results, the suspension process carried out pH controls that resulted in pH 11.15, 1.42, 3.86, and 4.55. The pH of the suspension affected the stability of the particle resistance, determine the direction and speed of migration during an electrophoretic deposition process. The pH controls also have affected the result of coating the structure between stainless steel 304 and Apatite compound becomes compact, uniform, and robust.
ACKNOWLEDGMENTS
The authors acknowledge the facilities and technical assistance from staff at Laboratory Material Physics and Instrumentation of UGM, Yogyakarta, Indonesia. The authors also would like to thank the Lembaga Penelitian dan Pengabdian pada Masyarakat, Universitas Kristen Indonesia Toraja (LPPM-UKI Toraja) for supporting this conference.
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