Enhancing Mechanical and Biocorrosion Response of a MgZnCa Bulk Metallic Glass through Variation in Spark Plasma Sintering Time
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Synthesis
2.3. Characterization
2.3.1. Surface Morphology
2.3.2. Density and Porosity
2.3.3. Mechanical Properties
2.3.4. Biocorrosion Tests
3. Results
3.1. Spark Plasma Sintering of Mg-Zn-Ca BMGs
3.2. Density and Porosity
3.3. Mechanical Properties
3.4. Biocorrosion Properties
4. Discussion
Influence of Sintering Time on the Densification of Melt-Spun Ribbons
5. Summary
- (1)
- Increasing the sintering time during the SPS process is effective in improving the density and structural integrity of Mg-Zn-Ca BMGs at 150 °C and 90 MPa.
- (2)
- A predominantly amorphous structure was obtained post SPS with a sintering time of up to 90 min (SPS150_90), with density close to that of the master alloy (2.82 g/cm3 vs. 2.85 g/cm3, ~98.2% densification). Densification increases with increasing sintering time.
- (3)
- SPS150_90 achieved UCS of 220 MPa, which is similar to that of cortical bone, thereby eliminating the issue of stress shielding.
- (4)
- Sintered samples with a sintering time of 90 min or less have similar corrosion resistance. There was a slight reduction in corrosion resistance (~2×) from SPS150_30 to SPS150_90 (0.214 mm/year vs. 0.394 mm/year). Nonetheless, SPS150_90 exhibited ~10× better corrosion resistance than as-cast MgZnCa (0.394 mm/year vs. 4.086 mm/year).
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
- González, S. Improved mechanical performance and delayed corrosion phenomena in biodegradable Mg–Zn–Ca alloys through Pd-alloying. J. Mech. Behav. Biomed. Mater. 2012, 6, 53–62. [Google Scholar] [CrossRef] [PubMed]
- Kraus, T.; Fischerauer, S.F.; Hänzi, A.C.; Uggowitzer, P.J.; Löffler, J.F.; Weinberg, A.M. Magnesium alloys for temporary implants in osteosynthesis: In vivo studies of their degradation and interaction with bone. Acta Biomater. 2012, 8, 1230–1238. [Google Scholar] [CrossRef]
- Lu, W.; He, M.; Yu, D.; Xie, X.; Wang, H.; Wang, S.; Yuan, C.; Chen, A. Ductile behavior and excellent corrosion resistance of Mg-Zn-Yb-Ag metallic glasses. Mater. Des. 2021, 210, 110027. [Google Scholar] [CrossRef]
- Babaremu, K.O.; John, M.E.; Mfoh, U.; Akinlabi, E.T.; Okokpujie, I.P. Behavioral Characteristics of Magnesium as a Biomaterial for Surface Engineering Application. J. Bio Tribo Corros. 2021, 7, 142. [Google Scholar] [CrossRef]
- Denkena, B.; Lucas, A. Biocompatible Magnesium Alloys as Absorbable Implant Materials—Adjusted Surface and Subsurface Properties by Machining Processes. CIRP Ann. 2007, 56, 113–116. [Google Scholar] [CrossRef]
- Bin, S.J.B.; Fong, K.S.; Chua, B.W.; Gupta, M. Mg-based bulk metallic glasses: A review of recent developments. J. Magnes. Alloys 2021, 10, 899–914. [Google Scholar] [CrossRef]
- Cai, A.H.; Xiong, X.; Yong, L.; An, W.K.; Zhou, G.J.; Yun, L.; Tie-Lin, L.; Li, X.S. Effect of consolidation parameters on mechanical properties of Cu-based bulk amorphous alloy consolidated by hot pressing. Trans. Nonferrous Met. Soc. China 2012, 22, 2032–2040. [Google Scholar] [CrossRef]
- Lee, P.Y.; Kao, M.C.; Lin, C.K.; Huang, J.C. Mg–Y–Cu bulk metallic glass prepared by mechanical alloying and vacuum hot-pressing. Intermetallics 2006, 14, 994–999. [Google Scholar] [CrossRef]
- Robertson, J.; Im, J.T.; Karaman, I.; Hartwig, K.T.; Anderson, I.E. Consolidation of amorphous copper based powder by equal channel angular extrusion. J. Non Cryst. Solids 2003, 317, 144–151. [Google Scholar] [CrossRef]
- Pauly, S. Processing metallic glasses by selective laser melting. Mater. Today 2013, 16, 37–41. [Google Scholar] [CrossRef]
- Bin, S.J.B.; Fong, K.S.; Chua, B.W.; Gupta, M. Development of Biocompatible Bulk MgZnCa Metallic Glass with Very High Corrosion Resistance in Simulated Body Fluid. Materials 2022, 15, 8989. [Google Scholar] [CrossRef] [PubMed]
- Anselmi-Tamburini, U. Spark Plasma Sintering. In Encyclopedia of Materials: Technical Ceramics and Glasses; Pomeroy, M., Ed.; Elsevier: Oxford, UK, 2021; pp. 294–310. [Google Scholar] [CrossRef]
- Cardinal, S.; Pelletier, J.M.; Qiao, J.C.; Bonnefont, G.; Xie, G. Influence of spark plasma sintering parameters on the mechanical properties of Cu50Zr45Al5 bulk metallic glass obtained using metallic glass powder. Mater. Sci. Eng. A 2016, 677, 116–124. [Google Scholar] [CrossRef]
- Zhang, Y.N.; Rocher, G.J.; Briccoli, B.; Kevorkov, D.; Liu, X.B.; Altounian, Z.; Medraj, M. Crystallization characteristics of the Mg-rich metallic glasses in the Ca–Mg–Zn system. J. Alloys Compd. 2013, 552, 88–97. [Google Scholar] [CrossRef]
- Jin, C.; Liu, Z.; Yu, W.; Qin, C.; Yu, H.; Wang, Z. Biodegradable Mg–Zn–Ca-Based Metallic Glasses. Materials 2022, 15, 2172. [Google Scholar] [CrossRef]
- Shamlaye, K.F.; Löffler, J.F. Synthesis and characterization of Mg-based bulk metallic glasses in the Mg–Ag–Y–(Cu) system. J. Alloys Compd. 2021, 859, 157803. [Google Scholar] [CrossRef]
- Yang, D.; Zhang, Y.; Song, X.; Chen, Y.; Shen, Z.; Yang, C. Effects of sintering temperature and holding time on porosity and shrinkage of glass tubes. Ceram. Int. 2016, 42, 5906–5910. [Google Scholar] [CrossRef]
- Muhammad, W.N.A.W.; Sajuri, Z.; Mutoh, Y.; Miyashita, Y. Microstructure and mechanical properties of magnesium composites prepared by spark plasma sintering technology. J. Alloys Compd. 2011, 509, 6021–6029. [Google Scholar] [CrossRef]
- Putra, A.G.; Manaf, A.; Anawati, A. Enhancing the Hardness of Mg-9Al-1Zn Cast Alloy by Solution Treatment. IOP Conf. Ser. Mater. Sci. Eng. 2019, 515, 012088. [Google Scholar] [CrossRef]
- Minarik, P.; Stráský, J.; Veselý, J.; Lukáč, F.; Hadzima, B.; Kral, R. AE42 magnesium alloy prepared by spark plasma sintering. J. Alloys Compd. 2018, 742, 172–179. [Google Scholar] [CrossRef]
- Morgan, E.F.; Unnikrisnan, G.U.; Hussein, A.I. Bone Mechanical Properties in Healthy and Diseased States. Annu. Rev. Biomed. Eng. 2018, 20, 119–143. [Google Scholar] [CrossRef]
- Be’ery-Lipperman, M.; Gefen, A. A method of quantification of stress shielding in the proximal femur using hierarchical computational modeling. Comput. Methods Biomech. Biomed. Engin. 2006, 9, 35–44. [Google Scholar] [CrossRef]
- Raffa, M.L.; Nguyen, V.H.; Hernigou, P.; Flouzat-Lachaniette, C.H.; Haiat, G. Stress shielding at the bone-implant interface: Influence of surface roughness and of the bone-implant contact ratio. J. Orthop. Res. 2021, 39, 1174–1183. [Google Scholar] [CrossRef] [PubMed]
- Leslie, N.; Mauzeroll, J. Spatially resolved electrochemical measurements. In Reference Module in Chemistry, Molecular Sciences and Chemical Engineering; Elsevier: Amsterdam, The Netherlands, 2023. [Google Scholar] [CrossRef]
- Chen, J.; Zhu, X.; Etim, I.P.; Siddiqui, M.A.; Su, X. Comparative study of the effects of MAO coating and Ca-P coating on the biodegradation and biocompatibility of Mg 69 Zn 27 Ca 4 metal glass. Mater. Technol. 2020, 37, 21–27. [Google Scholar] [CrossRef]
- Zhang, Y.; Yan, C.; Wang, F.; Li, W. Electrochemical behavior of anodized Mg alloy AZ91D in chloride containing aqueous solution. Corros. Sci. 2005, 47, 2816–2831. [Google Scholar] [CrossRef]
- Gu, X.; Zheng, Y.; Zhong, S.; Xi, T.; Wang, J.; Wang, W. Corrosion of, and cellular responses to Mg–Zn–Ca bulk metallic glasses. Biomaterials 2010, 31, 1093–1103. [Google Scholar] [CrossRef]
- Ford, D.C.; Hicks, D.; Oses, C.; Toher, C.; Curtarolo, S. Metallic glasses for biodegradable implants. Acta Mater. 2019, 176, 297–305. [Google Scholar] [CrossRef]
- Noviana, D.; Paramitha, D.; Ulum, M.F.; Hermawan, H. The effect of hydrogen gas evolution of magnesium implant on the postimplantation mortality of rats. J. Orthop. Transl. 2016, 5, 9–15. [Google Scholar] [CrossRef] [PubMed]
- Rybalka, K.V.; Beketaeva, L.A.; Davydov, A.D. Determination of corrosion current density by the rate of cathodic depolarizer consumption. Russ. J. Electrochem. 2016, 52, 268–272. [Google Scholar] [CrossRef]
- Balani, K.; Verma, V.; Agarwal, A.; Narayan, R. Corrosion Behavior of Metals. In Biosurfaces; John Wiley & Sons, Ltd.: New York, NY, USA, 2014; pp. 345–352. [Google Scholar] [CrossRef]
- Schmidt, H.; Gruber, W.; Gutberlet, T.; Ay, M.; Stahn, J.; Geckle, U.; Bruns, M. Structural relaxation and self-diffusion in covalent amorphous solids: Silicon nitride as a model system. J. Appl. Phys. 2007, 102, 043516. [Google Scholar] [CrossRef]
- Lee, D.; Vlassak, J.J. Diffusion kinetics in binary CuZr and NiZr alloys in the super-cooled liquid and glass states studied by nanocalorimetry. Scr. Mater. 2019, 165, 73–77. [Google Scholar] [CrossRef]
- Syutkin, V.M.; Grebenkin, S. Diffusion in bulk metallic glasses. Appl. Phys. Lett. 2020, 117, 134104. [Google Scholar] [CrossRef]
- Lazarus, D. Diffusion in Crystalline and Amorphous Solids. MRS Online Proc. Libr. (OPL) 1985, 57, 297. [Google Scholar] [CrossRef]
- Suárez, M.; Fernández-González, D.; Díaz, L.A.; Diologent, F.; Verdeja, L.F.; Fernández, A. Consolidation and mechanical properties of ZrCu39.85Y2.37Al1.8 bulk metallic glass obtained from gas-atomized powders by spark plasma sintering. Intermetallics 2021, 139, 107366. [Google Scholar] [CrossRef]
- Paul, T.; Singh, A.; Littrell, K.C.; Ilavsky, J.; Harimkar, S.P. Crystallization Mechanism in Spark Plasma Sintered Bulk Metallic Glass Analyzed using Small Angle Neutron Scattering. Sci. Rep. 2020, 10, 2033. [Google Scholar] [CrossRef]
- Zheng, B.; Ashford, D.; Zhou, Y.; Mathaudhu, S.N.; Delplanque, J.P.; Lavernia, E.J. Influence of mechanically milled powder and high pressure on spark plasma sintering of Mg–Cu–Gd metallic glasses. Acta Mater. 2013, 61, 4414–4428. [Google Scholar] [CrossRef]
- Perrière, L.; Champion, Y.; Bernard, F. Spark Plasma Sintering of Metallic Glasses. In Spark Plasma Sintering of Materials: Advances in Processing and Applications; Cavaliere, P., Ed.; Springer International Publishing: Cham, Switzerland, 2019; pp. 291–335. [Google Scholar] [CrossRef]
- Tyagi, A.K.; Macht, M.P.; Naundorf, V. Diffusion coefficients of 63Ni in Fe40Ni40B20 metallic glass. Acta Metall. Mater. 1991, 39, 609–617. [Google Scholar] [CrossRef]
- Perrière, L.; Thaï, M.T.; Tusseau-Nenez, S.; Ochin, P.; Blétry, M.; Champion, Y. Spark plasma sintering for metallic glasses processing. Rev. Métallurgie 2012, 109, 5–10. [Google Scholar] [CrossRef]
- Ajenifuja, E.; Odetola, P.; Popoola, A.P.; Popoola, O. Spark plasma sintering and structural analysis of nickel-titanium/coconut shell powder metal matrix composites. Int. J. Adv. Manuf. Technol. 2020, 108, 3465–3473. [Google Scholar] [CrossRef]
- Olson, G.L.; Roth, J.A. Kinetics of solid phase crystallization in amorphous silicon. Mater. Sci. Rep. 1988, 3, 1–77. [Google Scholar] [CrossRef]
- Yavari, A.R.; Le Moulec, A.; Inoue, A.; Nishiyama, N.; Lupu, N.; Matsubara, E.; José Botta, W.; Vaughan, G.; Di Michiel, M.; Kvick, Å. Excess free volume in metallic glasses measured by X-ray diffraction. Acta Mater. 2005, 53, 1611–1619. [Google Scholar] [CrossRef]
Raw Material | Supplier |
---|---|
Magnesium (Mg) turnings, 99.9% purity | ACROS Organics, Waltham, MA, USA |
Zinc (Zn) granules, 99.8% purity | Alfa Aesar, Waltham, MA, USA |
Calcium (Ca) granules, 99.8% purity | Alfa Aesar, Waltham, MA, USA |
Starting Temp (°C) | Heating Rate (°C/min) | Time (min) | Heating Rate (°C/min) | Time (min) | Final Temperature (°C) | Sintering Time (min) | Force (kN) | Pressure (MPa) | |
---|---|---|---|---|---|---|---|---|---|
SPS150_15 | 30 | 15 | 4 | 7 | 8.6 | 150 | 15 | 7 | 90 |
SPS150_30 | 30 | 15 | 4 | 7 | 8.6 | 150 | 30 | 7 | 90 |
SPS150_60 | 30 | 15 | 4 | 7 | 8.6 | 150 | 60 | 7 | 90 |
SPS150_90 | 30 | 15 | 4 | 7 | 8.6 | 150 | 90 | 7 | 90 |
SPS150_180 | 30 | 15 | 4 | 7 | 8.6 | 150 | 180 | 7 | 90 |
Material Composition | Raw Materials Composition by Weight % | Theoretical Density (g/cm3) | Actual Density (g/cm3) |
---|---|---|---|
Mg65Zn30Ca5 | Mg 42.2% Zn 52.42% Ca 5.36% | 2.86 | 2.85 |
Sample Name | UCS (MPa) | Reference |
---|---|---|
As-cast | 324 ± 10 | - |
Cortical bone | 205 ± 17 | [21] |
SPS150_15 | 108 ± 10.5 | - |
SPS150_30 | 143 ± 7.4 | - |
SPS150_60 | 187 ± 8.9 | - |
SPS150_90 | 220 ± 5.3 | - |
SPS150_180 | 254 ± 7.2 | - |
Sample Name | Icorr (mA/cm2) | Ecorr (mVSCE) | Corrosion Rate (mm/Year) |
---|---|---|---|
CRYSTALLINE | 19.2 × 10−2 | −1469 | 4.086 |
SPS150_15 | 1.25 × 10−2 | −1276 | 0.265 |
SPS150_30 | 1.01 × 10−2 | −1240 | 0.214 |
SPS150_60 | 1.95 × 10−2 | −1200 | 0.413 |
SPS150_90 | 1.86 × 10−2 | −1290 | 0.394 |
SPS150_180 | 3.91 × 10−2 | −1351 | 0.829 |
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Bryan, B.S.J.; Fong, K.S.; Wah, C.B.; Tekumalla, S.; Kwak, M.K.; Park, E.S.; Gupta, M. Enhancing Mechanical and Biocorrosion Response of a MgZnCa Bulk Metallic Glass through Variation in Spark Plasma Sintering Time. Metals 2023, 13, 1487. https://doi.org/10.3390/met13081487
Bryan BSJ, Fong KS, Wah CB, Tekumalla S, Kwak MK, Park ES, Gupta M. Enhancing Mechanical and Biocorrosion Response of a MgZnCa Bulk Metallic Glass through Variation in Spark Plasma Sintering Time. Metals. 2023; 13(8):1487. https://doi.org/10.3390/met13081487
Chicago/Turabian StyleBryan, Bin Shi Jie, Kai Soon Fong, Chua Beng Wah, Sravya Tekumalla, Min Kyung Kwak, Eun Soo Park, and Manoj Gupta. 2023. "Enhancing Mechanical and Biocorrosion Response of a MgZnCa Bulk Metallic Glass through Variation in Spark Plasma Sintering Time" Metals 13, no. 8: 1487. https://doi.org/10.3390/met13081487