Effect of corrosion product films on the in vitro degradation behavior of Mg-3%Al-1%Zn (in wt%) alloy in Hank’s solution

doi:10.1016/j.jmst.2018.02.013

Abstract

Abstract:

Through investigating the corrosion behavior of an as-extruded Mg-3wt%Al-1wt%Zn (AZ31) alloy in a simulated physiological fluid of Hank’s solution, it demonstrates that the corrosion process was dependent on the immersion time. Further analyses revealed that the highest corrosion resistance could be obtained at 24 h due to the formation of a compact layer of corrosion products on the sample surface. With increasing the immersion time to up to 48 h, the thickness of surface films increased gradually but obvious de-bonding of such film from the substrate could take place, resulting in a certain resilience of the overall corrosion resistance.

Key words: Magnesium, Surface layer, Corrosion product, Interface

B.J. Wang, D.K. Xu, J.H. Dong, W. Ke. Effect of corrosion product films on the in vitro degradation behavior of Mg-3%Al-1%Zn (in wt%) alloy in Hank’s solution[J]. J. Mater. Sci. Technol., 2018, 34(10): 1756-1764.

Figures/Tables 14

Fig. 1. XRD pattern of the as-extruded AZ31 alloy.

Fig. 2. Backscattered electron image of the as-extruded AZ31 alloy.

Fig. 3. Hydrogen evolution curve of the AZ31 alloy sample at the OCP in Hank’s solution.

Fig. 4. Representative potentiodynamic polarization curves of samples immersed in Hank’s solution for different time intervals.

Table 1 Fitting results of the polarization curves.

Conditions	i_corr (μA/cm²)	E_corr (V_SCE)
0.5 h	249.1 ± 36.5	1.47 ± 0.25
2 h	7.2 ± 2.0	1.48 ± 0.20
8 h	1.3 ± 0.2	1.45 ± 0.10
24 h	1.1 ± 0.1	1.35 ± 0.10
48 h	3.9 ± 0.5	1.43 ± 0.15

Fig. 5. Electrochemical impedance spectra of the samples after immersion in Hank’s solution for different time intervals: (a) Nyquist plots, (b) Bode plots of log |Z| vs logf and (c) Bode plots of phase angle vs logf.

Fig. 6. Equivalent circuit model representing two parallel time constants for an electrode/electrolyte interface.

Table 2 Fitting results of the EIS spectra.

Conditions	R_s (Ω cm²)	Y₀ (μΩ^-1 cm^-2sⁿ)	n	R₁ (Ω cm²)	C₁ (μF cm^-2)	R_f (Ω cm²)
0.5 h	20 ± 3	16.1 ± 0.5	0.66 ± 0.15	246 ± 30	1.3 ± 0.2	7902 ± 205
2 h	14 ± 1	18.3 ± 1.5	0.69 ± 0.15	90 ± 15	2.7 ± 0.5	10270 ± 537
8 h	18 ± 2	13.0 ± 0.5	0.68 ± 0.14	217 ± 26	2.4 ± 0.5	11350 ± 846
24 h	15 ± 1	42.4 ± 4.5	0.69 ± 0.15	346 ± 58	1.0 ± 0.1	16100 ± 975
48 h	19 ± 2	16.8 ± 0.5	0.68 ± 0.12	43 ± 5	1.8 ± 0.3	8224 ± 245

Fig. 7. Optical observations to the surfaces of samples after immersion in Hank’s solution for: (a) 0.5 h, (b) 2 h, (c) 8 h, (d) 16 h, (e) 24 h and (f) 48 h.

Fig. 8. Observations to the substrate surfaces of samples after immersion in Hank’s solution for: (a) 0.5 h, (b) 2 h, (c) 8 h, (d) 16 h, (e) 24 h and (f) 48 h. EDX results to the corroded surfaces are inserted in relevant images.

Fig. 9. XPS survey spectra of surface film of the sample immersed in Hank’s solution for 0.5 h after sputtering for 300 s.

Fig. 10. Elemental depth profiles of surface film of the sample immersed in Hank’s solution for 0.5 h.

Fig. 11. Typical XPS deconvolved spectra of surface film for the sample immersed in Hank’s solution for 0.5 h: (a) Mg-1s, (b) Ca-2s, (c) O-1 s and (d) P-2p.

Fig. 12. Cross-sectional microstructure of AZ31 alloy immersed in Hank’s solution for different time: (a) 2 h, (b) 8 h, (c) 24 h and (d) 48 h.

References

[1]	B.J. Wang, S.D. Wang, D.K. Xu, E.H. Han, J. Mater. Sci. Technol. 33(2017)1075-1086.
[2]	B.J. Wang, D.K. Xu, J.H. Dong, W. Ke, J. Mater. Sci. Technol. 32(2016) 646-652.
[3]	X.J. Wang, D.K. Xu, R.Z. Wu, X.B. Chen, Q.M. Peng, L. Jin, Y.C. Xin, Z.Q. Zhang, Y. Liu, X.H. Chen, G. Chen, K.K. Deng, H.Y. Wang, J. Mater. Sci. Technol. 34(2018)245-247.
[4]	P. Wan, L.L. Tan, K. Yang, J. Mater. Sci. Technol. 32(2016) 827-834.
[5]	P.F. Cheng, C.L. Zhao, P. Han, J.H. Ni, S.X. Zhang, X.N. Zhang, Y.M. Chai, J. Mater.Sci. Technol. 32(2016) 883-888.
[6]	C. Wang, H.T. Yang, X. Li, Y.F. Zheng, J. Mater. Sci. Technol. 32(2016) 909-918.
[7]	L.D. Hou, Z. Li, H. Zhao, Y. Pan, S. Pavlinich, X.W. Liu, X.L. Li, Y.F. Zheng, L. Li, J.Mater. Sci. Technol. 32(2016) 874-882.
[8]	T. Huang, Z.H. Wang, L.N. Wei, M. Kindy, Y.F. Zheng, T.F. Xi, B.Z. Gao, J. Mater.Sci. Technol. 32(2016) 89-96.
[9]	G.L. Song, Corros. Sci. 49(2007) 1696-1701.
[10]	R.C. Zeng, W. Dietzel, F. Witte, N. Hort, C. Blawert, Adv. Eng. Mater. 10(2008)3-14.
[11]	M.P. Staiger, A.M. Pietak, J. Huadmai, G. Dias, Biomaterials 27 (2006)1728-1734.
[12]	D.C. Xue, Y.H. Yun, M.J. Schulz, V. Shanov, Mater. Sci. Eng. C 31 (2011)215-223.
[13]	D.C. Xue, Y.H. Yun, Z.Q. Tan, Z.Y. Dong, M.J. Schulz, J. Mater, Sci. Technol. 28(2012) 261-267.
[14]	A. Hartwig, Mutat. Res.-Fundam. Mol. Mech. 475(2001) 113-121.
[15]	X.F. Cui, Y.Y. Yang, E.B. Liu, G. Jin, J.G. Zhong, Q.F. Li, Appl. Surf. Sci. 257(2011)9703-9709.
[16]	F. Witte, V. Kaese, H. Haferkamp, E. Switzer, A. Meyer-Lindenberg, C.J. Wirth,H. Windhagen, Biomaterials 26 (2005) 3557-3563.
[17]	C.E. Wen, M. Mabuchi, Y. Yamada, K. Shimojima, Y. Chino, T. Asahina, Scr.Mater. 45(2001) 1147-1153.
[18]	J. Levesque, H. Hermawan, D. Dube, D. Mantovani, Acta Biomater. 4(2008)284-295.
[19]	G. Han, J.Y. Lee, Y.C. Kim, J.H. Park, D.I. Kim, H.S. Han, S.J. Yang, H.K. Seok,Corros. Sci. 63(2012) 316-322.
[20]	L. Li, J. Gao, Y. Wang, Surf. Coat. Technol. 185(2004) 92-98.
[21]	Y. Xin, T. Hu, P.K. Chu, Acta Biomater. 7(2011) 1452-1459.
[22]	A.C. H?nzi, I. Gerber, M. Schinhammer, J.F. L?ffler, P.J. Uggowitzer, ActaBiomater. 6(2010) 1824-1833.
[23]	F. Witte, J. Fischer, J. Nellesen, H. Crostack, V. Kaese, A. Pisch, F. Beckmann, H. Windhagen, Biomaterials 27 (2006) 1013-1018.
[24]	A. Atrens, M. Liu, N.I. Zainal Abidin, Mater. Sci. Eng. B 176 (2011) 1609-1636.
[25]	F. Witte, N. Hort, C. Vogt, S. Cohen, K.U. Kainer, R. Willumeit, F. Feyerabend,Curr. Opin. Solid State Mater.Sci. 12(2008) 63-72.
[26]	A. Zomorodian, F. Brusciotti, A. Fernandes, M.J. Carmezim, T. Moura Silva, J.C.S. Fernandes, M.F. Montemor, Surf. Coat. Technol. 206(2012) 4368-4375.
[27]	Y.C. Xin, C.L. Liu, X.M. Zhang, G.Y. Tang, X.B. Tian, P.K. Chu, J. Mater. Res. 22(2007) 2004-2011.
[28]	Y.C. Xin, T. Hu, P.K. Chu, J. Electrochem. Soc. 157(2010) 238-243.
[29]	Y.C. Xin, K.F. Huo, T. Hu, G.Y. Tang, P.K. Chu, J. Mater. Res. 24(2009)2711-2719.
[30]	G.L. Song, A. Atrens, Adv. Eng. Mater. 5(2003) 837-858.
[31]	R. Rettig, S. Virtanen, J. Biomed, Mater. Res. A 88 (2009) 359-369.
[32]	L. Yang, E.L. Zhang, Mater. Sci. Eng. C 29 (2009) 1691-1696.
[33]	M. Ascencio, M. Pekguleryuz, S. Omanovic, Corros. Sci. 87(2014)489-503.
[34]	J. Kamran, U.D. Shamas, N.H. Tariq, F. Ali, B.A. Hasan, Mater. Des. 81(2015)11-20.
[35]	X. Xie, J. Shen, L. Cheng, Y. Li, Y.Y. Pu, Mater. Des. 81(2015) 31-38.
[36]	M. Saravanan, B. Sivaiah, A.K. Srivastava, A. Dhar, Mater. Des. 60(2014) 21-25.
[37]	L.W.F. Mackenzie, M. Pekguleryuzs, Mater. Sci. Eng. A 480 (2008) 189-197.
[38]	Z.B. Sajuri, Y. Miyashita, Y. Hosokai, Y. Mutohs, Int. J. Mech. Sci. 48(2006)198-209.
[39]	Alloy phase diagrams, in: ASM Handbook ASM International, vol. 3, 1992, pp.1535-1536.
[40]	M.C. Zhao, M. Liu, G.L. Song, A. Atrens, Corros. Sci. 50(2008) 3168-3178.
[41]	G. Wu, Y. Zhao, X. Zhang, J.M. Ibrahim, P.K. Chu, Corros. Sci. 68(2013)279-285.
[42]	X.W. Guo, J.W. Chang, S.M. He, W.J. Ding, X. Wang, Electrochim. Acta 52(2007) 2570-2579.
[43]	G. Baril, C. Blauc, N. Pebérè, J. Electrochem. Soc. 148(2001) 489-496.
[44]	A. Alabbasi, S. Liyanaarachchi, M.B. Kannan, Thin Solid Films 320 (2012)6841-6844.
[45]	F. El-Taib Heakal, O.S. Shehata, N.S. Tantawy, Corros. Sci. 86(2014) 285-294.
[46]	C.S. Wu, Z. Zhang, F.H. Cao, L.J. Zhang, J.Q. Zhang, C.N. Cao, Appl. Surf. Sci. 253(2007) 3893-3898.
[47]	R. Amini, A.A. Sarabi, Appl. Surf. Sci. 257(2011) 7134-7139.
[48]	L.J. Zhang, J.J. Fan, Z. Zhang, F.H. Cao, J.Q. Zhang, C.N. Cao, Electrochim. Acta 52(2007) 5325-5333.
[49]	C.N. Cao, J.Q. Zhang, Introduction of Electrochemical Impedance Spectroscopy, First ed., Science Press, Beijing, 2002.
[50]	Y. Zong, G.Y. Yuan, X.B. Zhang, L. Min, J.L. Niu, W.J. Ding, Mater. Sci. Eng. B 177(2012) 395-401.
[51]	Y.W. Song, D.Y. Shan, R.S. Chen, F. Zhang, E.H. Han, Mater. Sci. Eng. C 29 (2009)1039-1045.
[52]	Beijing Normal University, Inorganic Chemistry, Higher Education Press, Beijing, 2002.
[53]	C.Y. Zhang, R.C. Zeng, C.L. Liu, J.C. Gao, Surf. Coat. Technol. 204(2010)3636-3640.
[54]	J. Chen, J.Q. Wang, E.H. Han, J.H. Dong, W. Ke, Electrochim. Acta 52 (2007)3299-3309.
[55]	F.E.T. Heakal, A.M. Fekry, M.Z. Fatayerji, Electrochim. Acta 54 (2009)1545-1557.