Electrophoretic deposition of hydroxyapatite-iron oxide-chitosan composite coatings on Ti–13Nb–13Zr alloy for biomedical applications
Introduction
During the last decades, there is an increasing demand for replacement of damaged bones or hard tissues because of various diseases like osteoarthritis (inflammation in the joints of bone) [1], osteoporosis (weakening of the bones) [2], dentistry [3] and war-related injuries [4]. For this purpose, the biomaterials are widely used to regenerate the skeletal tissues in the body. Presently, the biomaterials used for dental and orthopedic applications are Titanium (Ti) based alloys, Stainless steel, Magnesium based alloys and Cobalt chromium alloys [5]. Among these biomaterials, Ti-based alloys proved to be the relevant material for their better corrosion resistance, attractive biocompatibility, moderate elastic modulus and favorable strength to weight ratio [6]. Moreover, in various fields such as osteosynthesis, oral implantology and joint prosthetics Ti alloys have exhibited their potential as an implant material [7]. In biomedical engineering, generally two phases (α + β) such as Ti–6Al–4V and Ti–6Al–7Nb alloys have been broadly employed as metallic implants but their long term use causes a stress shielding problem due to their biochemical incompatibility issues [8]. These two particular alloys contain vanadium and aluminum compounds that release toxic ions and produce adverse health effects [9]. Vanadium causes cytotoxicity whereas neurological disorder (Alzheimer's disease) is caused by aluminum [10]. Therefore, current studies have been focused on β alloys (Zr, Nb, Ta and Mo as alloy additives) which possesses better properties such as good ductility, similar mechanical strength, enhanced corrosion resistance and lower elastic modulus as compared to Ti–6Al–4V alloy [11,12]. The Nb and Zr into Ti are more biocompatible than V and Al and govern to the formation of β alloy structure [13].
In spite of all these features, Ti-based alloys are incapable to induce bone formation on their surface as they are classified as bioinert material. Moreover, implant failure occurs as there is insufficient growth of bone tissues [14]. Therefore, to improve the osseointegration phenomena various surface modifications have been done on Ti-based alloys. Among these surface modifications, HA has proved to be a potential candidate for bone tissue applications. HA boosts osteoconductivity and cell responses as it possesses similar compositional resemblance and crystal structure to that of human bone [15]. Moreover, HA coating helps to reduce the Ti-body fluid contact because of their good interfacial bond to Ti alloy substrate [16]. Various methods such as the sol-gel method [17], electrochemical method [18], plasma spray method [19] and electrophoretic deposition [20] were engaged to achieve the HA coating. Among these methods, EPD has shown more interest as it could be operated under atmospheric pressure and relatively low processing temperature [21]. As a contrast to other coating methods, EPD has many advantages such as low cost, simplicity, control the coating thickness, high production rates and ability to coat a substrate with intricate shapes [22], [23], [24].
Reportedly, implant failure occurs due to the high degradation rate of pure HA coating, which reduces the long term survivability of the implants in the body environment [25]. Huang et al. [26] demonstrated that the reinforced- HA coating has better potential to enhance the life of the implant than pure HA coating. To improve the properties of HA coating several reinforcements had been studied in combination with ceramic and polymer phases such as titanium oxide [27], silica oxide [28], iron oxide [29], zinc oxide [30], polycaprolactide [31], chitosan [32] and polylactide [33]. However, there is a growing interest for the Fe3O4 particles among the research community for their excellent characteristics such as tissue repair, small size, good mass transfer efficiency, the high surface area, non-toxicity, biocompatibility, easy preparation, cell imaging, drug delivery and purification of cell populations [34], [35], [36], [37]. In addition, Fe3O4 particles play a vital role in various in vitro and in vivo applications [38].
In order to refine the mechanical and biological behavior of inorganic composite materials, a great deal of interest is focused on organic polymer coatings [39]. Among the organic materials, chitosan acts as a capping agent due to their remarkable properties such as wound healing activity, biocompatibility, biodegradability, antibacterial and environmental friendliness [40], [41], [42]. CS is a naturally occurring polysaccharide which strongly interacts with negatively charged bodies [43]. Moreover, the utilization of CS vanish the disadvantage of high-temperature and prevent the substrate from micro-cracking and shrinkage [44]. In the earlier study, it has been suggested that the corrosion resistance and biological performance was improved by CS composite coatings on Ti substrate [45]. Yadav et al. [46] prepared the composites by utilizing the combination of metal oxide particles and CS. It was observed that the biocompatibility and surface properties were improved by incorporation of Fe3O4 particles. Due to the presence of amine groups, CS provides a hydrophilic environment which is more compatible for the biomolecules [47]. Therefore, reinforcement of Fe3O4 as a secondary phase in HA and CS composite coating is a favorable approach to enhance the surface properties as well as corrosion resistance.
In the present investigation, the Ti–13Nb–13Zr alloy was electrophoretically coated with pure HA, pure Fe3O4 and HA–Fe3O4–CS coatings by altering the concentration of Fe3O4 at three different levels i.e. 1, 3 and 5 wt%. As per literature available, the findings of corrosion resistance and analysis of surface properties of EPD coated Fe3O4 particles with HA and chitosan-based coatings on the Ti–13Nb–13Zr alloy are yet to be established. In addition, the bioactivity behavior, surface roughness and wettability of the samples were observed and discussed.
Section snippets
Materials
The chemicals used for experimental work are as follow: Iron sulphate (FeSO4) and Ferric trichloride hexahydrate (FeCl3) (Micro X Labs, India), Chitosan with MW = 85 kDa (Sisco Research Lab, India), Nitric acid, Hydrochloric acid, Ammonium hydroxide, Acetic acid, Sulfuric acid, Acetone, Ethanol, Deionized water (DI) (Loba Chemie Pvt. Ltd., India). Hydroxyapatite nanopowder used as the coating material (Trixotech Advanced Materials Pvt. Ltd. India). The Ti–13Nb–13Zr alloy (13.00 Nb, 13.50 Zr,
Results and discussion
EPD is generally conducted in a two-electrode cell and based on electrophoresis mechanism. The migration of charged particles between the electrodes initiates due to the existence of an electric field in the suspension [59]. The formation of the suspension and the EPD process was shown in Fig. 1.
The measurement of zeta potential showed the good dispersion, suspension stability and direction to charged particles movement in suspension [60]. In order to check suspension stability, the zeta
Conclusions
In this study, HA- Fe3O4-CS composite coatings were successfully developed by the EPD over Ti–13Nb–13Zr alloy. The incorporation of Fe3O4 into HA-CS increase the stability of the suspension and stimulate the HA deposition. The composite coatings exhibited good crystallinity as compared to the HA coating. The SEM micrographs revealed crack-free and uniform coating with micropores on the surface. The composite coatings fabricated by EPD showed better rough surfaces that tend to a significant
Funding
This research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors.
CRediT authorship contribution statement
Sandeep Singh: Conceptualization, Methodology, Writing - original draft, Visualization, Investigation. Gurpreet Singh: Supervision, Writing - review & editing, Conceptualization. Niraj Bala: Formal analysis, Writing - review & editing.
Declaration of Competing Interest
The authors declarae that they have known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgment
The authors are thankful to the Indian Institute of Technology Ropar, India for experimental facilities.
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