J. Mater. Sci. Technol. ›› 2020, Vol. 46: 33-43.DOI: 10.1016/j.jmst.2019.10.043
• Research Article • Previous Articles Next Articles
Zhangweijia Qiua,b, Zhengkun Lib, Huameng Fub,d,*(), Hongwei Zhangb,c,d, Zhengwang Zhub,d, Aimin Wangb,d, Hong Lib, Long Zhangb, Haifeng Zhangb,d,*()
Received:
2019-08-26
Revised:
2019-09-27
Accepted:
2019-10-25
Published:
2020-06-01
Online:
2020-06-19
Contact:
Huameng Fu,Haifeng Zhang
Zhangweijia Qiu, Zhengkun Li, Huameng Fu, Hongwei Zhang, Zhengwang Zhu, Aimin Wang, Hong Li, Long Zhang, Haifeng Zhang. Corrosion mechanisms of Zr-based bulk metallic glass in NaF and NaCl solutions[J]. J. Mater. Sci. Technol., 2020, 46: 33-43.
Fig. 1. Microstructure characterizations for as-cast Zr52Al10Ni6Cu32 BMG sample: (a) XRD pattern; (b) HRTEM image with the corresponding SAED pattern in the inset.
Fig. 2. Variations of open circuit potentials with time for Zr52Al10Ni6Cu32 metallic glass in electrolytes: (a) NaCl solutions; (b) NaF solutions, and the results of subsequent EIS tests with equivalent circuit used to fit data: (c) NaCl solutions; (d) NaF solutions.
NaCl Solution | Rs (Ω cm2) | CPE (μS sn cm-2) | n | Rf (kΩ cm2) | Rp (kΩ cm2) | χ2(×10-4) | |||
---|---|---|---|---|---|---|---|---|---|
0.05 M | 2.66 | 13.61 | 0.91 | 556.4 | 556.4 | 2.18 | |||
0.1 M | 2.66 | 14.13 | 0.91 | 508.2 | 508.2 | 2.38 | |||
0.2 M | 2.26 | 14.51 | 0.9 | 483.3 | 483.3 | 1.24 | |||
0.5 M | 2.38 | 12.77 | 0.93 | 428.7 | 428.7 | 1.76 | |||
NaF Solution | Rs (Ω cm2) | CPE1 (μS sn cm-2) | n1 | Rf1 (kΩ cm2) | CPE2 (μS sn cm-2) | n2 | Rf2 (kΩ cm2) | Rp (kΩ cm2) | χ2 |
0.05 M | 13.34 | 14.32 | 0.91 | 28.1 | 10.02 | 0.91 | 141.1 | 170.2 | 6.77 |
0.1 M | 12.59 | 14.05 | 0.93 | 20.4 | 10.61 | 0.93 | 64.1 | 84.5 | 8.42 |
0.2 M | 7.65 | 15.54 | 0.93 | 10.7 | 28.37 | 0.81 | 27 | 37.7 | 9.79 |
0.5 M | 5.01 | 27.33 | 0.93 | 1.2 | 31.69 | 0.81 | 3.7 | 4.9 | 9.54 |
Table 1 Values of impedance parameters of EIS experiments obtained by fitting for Zr-based metallic glass after open circuit potential tests.
NaCl Solution | Rs (Ω cm2) | CPE (μS sn cm-2) | n | Rf (kΩ cm2) | Rp (kΩ cm2) | χ2(×10-4) | |||
---|---|---|---|---|---|---|---|---|---|
0.05 M | 2.66 | 13.61 | 0.91 | 556.4 | 556.4 | 2.18 | |||
0.1 M | 2.66 | 14.13 | 0.91 | 508.2 | 508.2 | 2.38 | |||
0.2 M | 2.26 | 14.51 | 0.9 | 483.3 | 483.3 | 1.24 | |||
0.5 M | 2.38 | 12.77 | 0.93 | 428.7 | 428.7 | 1.76 | |||
NaF Solution | Rs (Ω cm2) | CPE1 (μS sn cm-2) | n1 | Rf1 (kΩ cm2) | CPE2 (μS sn cm-2) | n2 | Rf2 (kΩ cm2) | Rp (kΩ cm2) | χ2 |
0.05 M | 13.34 | 14.32 | 0.91 | 28.1 | 10.02 | 0.91 | 141.1 | 170.2 | 6.77 |
0.1 M | 12.59 | 14.05 | 0.93 | 20.4 | 10.61 | 0.93 | 64.1 | 84.5 | 8.42 |
0.2 M | 7.65 | 15.54 | 0.93 | 10.7 | 28.37 | 0.81 | 27 | 37.7 | 9.79 |
0.5 M | 5.01 | 27.33 | 0.93 | 1.2 | 31.69 | 0.81 | 3.7 | 4.9 | 9.54 |
Fig. 3. Typical SEM images of Zr52Al10Ni6Cu32 metallic glass samples after open circuit potential tests in 0.2 M NaCl (a), 0.5 M NaCl (b), 0.2 M NaF (c), and 0.5 M NaF (d).
NaCl | NaF | |||||
---|---|---|---|---|---|---|
Ecorr (mV vs SCE) | Epit (mV vs SCE) | icorr (μA/cm2) | Ecorr (mV vs SCE) | Eb (mV vs SCE) | icorr (μA/cm2) | |
0.05 M | -257 ± 28 | -19 ± 59 | 164 ± 14 | -184 ± 46 | 529 ± 74 | 168.6 ± 21 |
0.1 M | -291 ± 43 | -46 ± 53 | 169 ± 8 | -225 ± 29 | 243 ± 61 | 292.1 ± 19 |
0.2 M | -317.3 ± 19 | -139 ± 30 | 178 ± 15 | -249 ± 34 | -40.0 ± 41 | 383.9 ± 60 |
0.5 M | -332.9 ± 33 | -204 ± 59 | 201 ± 38 | -289 ± 26 | -149.8 ± 57 | 732.2 ± 116 |
Table 2 Electrochemical parameters obtained from the polarization curves of Zr52Al10Ni6Cu32 BMG samples in NaCl and NaF solution.
NaCl | NaF | |||||
---|---|---|---|---|---|---|
Ecorr (mV vs SCE) | Epit (mV vs SCE) | icorr (μA/cm2) | Ecorr (mV vs SCE) | Eb (mV vs SCE) | icorr (μA/cm2) | |
0.05 M | -257 ± 28 | -19 ± 59 | 164 ± 14 | -184 ± 46 | 529 ± 74 | 168.6 ± 21 |
0.1 M | -291 ± 43 | -46 ± 53 | 169 ± 8 | -225 ± 29 | 243 ± 61 | 292.1 ± 19 |
0.2 M | -317.3 ± 19 | -139 ± 30 | 178 ± 15 | -249 ± 34 | -40.0 ± 41 | 383.9 ± 60 |
0.5 M | -332.9 ± 33 | -204 ± 59 | 201 ± 38 | -289 ± 26 | -149.8 ± 57 | 732.2 ± 116 |
Fig. 5. Typical SEM images and corresponding EDS results of selected areas in Zr52Al10Ni6Cu32 BMG sample after pitting in 0.1 M NaCl solution: (a) Image of corroded surface; (b) High-resolution image of corrosion pit; (c) EDS results of area A; (d) EDS resuls of area B.
Fig. 6. Optical micrographs of polarization process of Zr52Al10Ni6Cu32 BMG samples in 0.1 M NaF solution: (a-d) and corresponding polarization curves (e-h).
Ionic radii (nm)a | Surface charge density (mC/m2) | B((L/mol)b | |
---|---|---|---|
F- | 0.133 | 720.16 | 0.1 |
Cl- | 0.181 | 388.84 | -0.007 |
OH- | 0.133 | 720.16 | - |
Zr4+ | 0.072 | 9824.67 | - |
Na+ | 0.102 | 1223.84 | 0.086 |
Table 3 Ionic radii, surface charge densities, and viscosity B coefficients of ions.
Ionic radii (nm)a | Surface charge density (mC/m2) | B((L/mol)b | |
---|---|---|---|
F- | 0.133 | 720.16 | 0.1 |
Cl- | 0.181 | 388.84 | -0.007 |
OH- | 0.133 | 720.16 | - |
Zr4+ | 0.072 | 9824.67 | - |
Na+ | 0.102 | 1223.84 | 0.086 |
log β1 | log β2 | log β3 | log β4 | |
---|---|---|---|---|
Chloridea | 0.9 | 1.3 | 1.5 | 1.2 |
Fluorideb | 5.84 | 10.23 | 13.12 | 15.30 |
Hydroxidea | 14.3 | 28.3 | 41.9 | 55.3 |
Table 4 Cumulative formation constants of zirconium cation with chloride, fluoride and hydroxide.
log β1 | log β2 | log β3 | log β4 | |
---|---|---|---|---|
Chloridea | 0.9 | 1.3 | 1.5 | 1.2 |
Fluorideb | 5.84 | 10.23 | 13.12 | 15.30 |
Hydroxidea | 14.3 | 28.3 | 41.9 | 55.3 |
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