J. Mater. Sci. Technol. ›› 2021, Vol. 64: 38-56.DOI: 10.1016/j.jmst.2020.03.031
• Research article • Previous Articles Next Articles
Dawei Guoa, Chi Tat Kwoka,b,*(
)
Received:2020-02-23
Accepted:2020-03-20
Published:2021-02-20
Online:2021-03-15
Contact:
Chi Tat Kwok
About author:*Department of Electromechanical Engineering, Uni-versity of Macau, Macau, ChinaE-mail address: fstctk@um.edu.mo (C.T. Kwok).Dawei Guo, Chi Tat Kwok. A corrosion study on W-Cu alloys in sodium chloride solution at different pH[J]. J. Mater. Sci. Technol., 2021, 64: 38-56.
Fig. 1. (a) The combined Pourbaix diagrams of W-Cl-H2O and Cu-Cl-H2O systems. (b) The combined Pourbaix diagrams of W-H2O and Cu-H2O systems.
Fig. 2. Microstructures of (a) cp Cu (etched with the ferric chloride solution, 5 g FeCl3, 30 mL HCl and 100 mL distilled water), (b) cp W (electrochemically etched with 1 mol/L NaOH solution), (c) W80Cu20 and (d) W90Cu10.
Fig. 3. Time dependence of (a, c) galvanic potential and (b, d) galvanic current density for galvanic couples of cp Cu vs cp W in water with (a, b) and without (c, d) 3.38 wt.% NaCl at pH 1, 7 and 13.
| Average galvanic potential (VSCE) | Average galvanic current density (μA/cm2) | |
|---|---|---|
| pH1 | -0.2 | -13 |
| pH7 | -0.25 | 1 |
| pH13 | -0.5 | 33 |
Table 1 Average galvanic potentials and galvanic current densities for the galvanic couples (cp Cu and cp W) attained at various pH with 3.38 wt.% NaCl after 7 days.
| Average galvanic potential (VSCE) | Average galvanic current density (μA/cm2) | |
|---|---|---|
| pH1 | -0.2 | -13 |
| pH7 | -0.25 | 1 |
| pH13 | -0.5 | 33 |
| OCP/Ecorr-DP (VSCE) | icorr (μA/cm2) | Epit (VSCE) | |
|---|---|---|---|
| cp Cu | |||
| pH 1 | -0.3 | 1.5 | 0.06 |
| pH 3 | -0.3 | 0.8 | 0.02 |
| pH 7 | -0.2 | 0.9 | 0.02 |
| pH 11 | -0.2 | 1.0 | - |
| pH 13 | -0.2 | 1.3 | 0.13 |
| W80Cu20 direct polarization (DP) | |||
| pH 1 | -0.2 | 18.9 | -0.03 |
| pH 3 | -0.3 | 2.3 | -0.02 |
| pH 7 | -0.4 | 3.8 | -0.02 |
| pH 11 | -0.5 | 8.2 | -0.01 |
| pH 13 | -0.5 | 17.2 | - |
| W90Cu10 direct polarization (DP) | |||
| pH 1 | -0.2 | 13.1 | -0.02 |
| pH 3 | -0.3 | 2.3 | -0.01 |
| pH 7 | -0.4 | 3.1 | -0.01 |
| pH 11 | -0.5 | 6.0 | -0.01 |
| pH 13 | -0.6 | 22.6 | - |
| cp W | |||
| pH 1 | -0.2 | 0.8 | - |
| pH 3 | -0.3 | 0.9 | - |
| pH 7 | -0.4 | 1.7 | - |
| pH 11 | -0.5 | 2.6 | active |
| pH 13 | -0.6 | 4.6 | active |
Table 2 Corrosion parameters of cp Cu, cp W, W80Cu20 and W90Cu10 in the solutions with 3.38 wt.% NaCl at various pH.
| OCP/Ecorr-DP (VSCE) | icorr (μA/cm2) | Epit (VSCE) | |
|---|---|---|---|
| cp Cu | |||
| pH 1 | -0.3 | 1.5 | 0.06 |
| pH 3 | -0.3 | 0.8 | 0.02 |
| pH 7 | -0.2 | 0.9 | 0.02 |
| pH 11 | -0.2 | 1.0 | - |
| pH 13 | -0.2 | 1.3 | 0.13 |
| W80Cu20 direct polarization (DP) | |||
| pH 1 | -0.2 | 18.9 | -0.03 |
| pH 3 | -0.3 | 2.3 | -0.02 |
| pH 7 | -0.4 | 3.8 | -0.02 |
| pH 11 | -0.5 | 8.2 | -0.01 |
| pH 13 | -0.5 | 17.2 | - |
| W90Cu10 direct polarization (DP) | |||
| pH 1 | -0.2 | 13.1 | -0.02 |
| pH 3 | -0.3 | 2.3 | -0.01 |
| pH 7 | -0.4 | 3.1 | -0.01 |
| pH 11 | -0.5 | 6.0 | -0.01 |
| pH 13 | -0.6 | 22.6 | - |
| cp W | |||
| pH 1 | -0.2 | 0.8 | - |
| pH 3 | -0.3 | 0.9 | - |
| pH 7 | -0.4 | 1.7 | - |
| pH 11 | -0.5 | 2.6 | active |
| pH 13 | -0.6 | 4.6 | active |
Fig. 4. XRD patterns of W80Cu20 after polarization test in 3.38 wt.% NaCl solution at various pH.
Fig. 5. (a, c) Plots of OCP vs time and (b, d) polarization curves in 3.38 wt.% NaCl solution at (a, b) pH 1 and (c, d) pH 3; SEM micrographs of corroded surface of W80Cu20 in 3.38 wt.% NaCl solutions at (e) pH 1 and (f) pH 3 after polarization test; SEM micrograph of corroded surface of W80Cu20 in water at pH 3 (g) after polarization test.
Fig. 6. SEM micrographs of (a) cp Cu (b) and cp W in 3.38 wt.% NaCl solution at pH 1 immersed for 31 days; SEM micrograph of (c) cp Cu in water at pH 1 immersed for 31 days.
Fig. 7. SEM micrographs of W80Cu20 in water at pH1 immersed for (a) 3, (b) 13 and (c) 31 days with (d) XRD pattern; (e) SEM micrograph of the detached tungsten particles; and (f) corrosion rate vs immersion time of cp Cu, cp W, W80Cu20 and W90Cu10 in 3.38 wt.% NaCl solution at pH 1.
| Cu (mol/L) | W (mol/L) | Cl (mol/L) | Na (mol/L) | pH | |
|---|---|---|---|---|---|
| Cu pH1 NaCl | 2.18 × 10-2 | - | 5.98 × 10-1 | 5.98 × 10-1 | 1.32 |
| Cu pH7 NaCl | 1.89 × 10-6 | - | 5.99 × 10-1 | 6.01 × 10-1 | 5.64 |
| Cu pH11 NaCl | 9.91 × 10-5 | - | 5.71 × 10-1 | 6.00 × 10-1 | 6.24 |
| Cu pH13 NaCl | N.D | - | 6.00 × 10-1 | 6.00 × 10-1 | 12.53 |
| W80Cu20 pH1 NaCl | 2.54 × 10-2 | 2.23 × 10-4 | 5.77 × 10-1 | 5.99 × 10-1 | 1.71 |
| W80Cu20 pH7 NaCl | 8.73 × 10-5 | 1.55 × 10-4 | 5.67 × 10-1 | 5.97 × 10-1 | 4.98 |
| W80Cu20 pH11 NaCl | 3.15 × 10-6 | 5.87 × 10-4 | 5.54 × 10-1 | 6.01 × 10-1 | 6.86 |
| W80Cu20 pH13 NaCl | 4.72 × 10-6 | 1.17 × 10-3 | 5.57 × 10-1 | 6.04 × 10-1 | 12.61 |
| W90Cu10 pH1 NaCl | 3.43 × 10-2 | 1.99 × 10-5 | 5.83 × 10-1 | 6.00 × 10-1 | 1.96 |
| W90Cu10 pH7 NaCl | 8.81 × 10-5 | 4.55 × 10-4 | 5.65 × 10-1 | 5.97 × 10-1 | 4.98 |
| W90Cu10 pH11 NaCl | 3.93 × 10-6 | 4.06 × 10-4 | 5.61 × 10-1 | 6.01 × 10-1 | 6.58 |
| W90Cu10 pH13 NaCl | N.D | 1.11 × 10-3 | 5.88 × 10-1 | 6.04 × 10-1 | 12.7 |
| W pH1 NaCl | - | 1.35 × 10-4 | 6.01 × 10-1 | 6.01 × 10-1 | 1.16 |
| W pH7 NaCl | - | 1.71 × 10-4 | 6.00 × 10-1 | 6.00 × 10-1 | 5.45 |
| W pH13 NaCl | - | 1.08 × 10-3 | 6.01 × 10-1 | 6.02 × 10-1 | 12.72 |
Table 3 Element concentration of solutions after immersion test measured by AAS.
| Cu (mol/L) | W (mol/L) | Cl (mol/L) | Na (mol/L) | pH | |
|---|---|---|---|---|---|
| Cu pH1 NaCl | 2.18 × 10-2 | - | 5.98 × 10-1 | 5.98 × 10-1 | 1.32 |
| Cu pH7 NaCl | 1.89 × 10-6 | - | 5.99 × 10-1 | 6.01 × 10-1 | 5.64 |
| Cu pH11 NaCl | 9.91 × 10-5 | - | 5.71 × 10-1 | 6.00 × 10-1 | 6.24 |
| Cu pH13 NaCl | N.D | - | 6.00 × 10-1 | 6.00 × 10-1 | 12.53 |
| W80Cu20 pH1 NaCl | 2.54 × 10-2 | 2.23 × 10-4 | 5.77 × 10-1 | 5.99 × 10-1 | 1.71 |
| W80Cu20 pH7 NaCl | 8.73 × 10-5 | 1.55 × 10-4 | 5.67 × 10-1 | 5.97 × 10-1 | 4.98 |
| W80Cu20 pH11 NaCl | 3.15 × 10-6 | 5.87 × 10-4 | 5.54 × 10-1 | 6.01 × 10-1 | 6.86 |
| W80Cu20 pH13 NaCl | 4.72 × 10-6 | 1.17 × 10-3 | 5.57 × 10-1 | 6.04 × 10-1 | 12.61 |
| W90Cu10 pH1 NaCl | 3.43 × 10-2 | 1.99 × 10-5 | 5.83 × 10-1 | 6.00 × 10-1 | 1.96 |
| W90Cu10 pH7 NaCl | 8.81 × 10-5 | 4.55 × 10-4 | 5.65 × 10-1 | 5.97 × 10-1 | 4.98 |
| W90Cu10 pH11 NaCl | 3.93 × 10-6 | 4.06 × 10-4 | 5.61 × 10-1 | 6.01 × 10-1 | 6.58 |
| W90Cu10 pH13 NaCl | N.D | 1.11 × 10-3 | 5.88 × 10-1 | 6.04 × 10-1 | 12.7 |
| W pH1 NaCl | - | 1.35 × 10-4 | 6.01 × 10-1 | 6.01 × 10-1 | 1.16 |
| W pH7 NaCl | - | 1.71 × 10-4 | 6.00 × 10-1 | 6.00 × 10-1 | 5.45 |
| W pH13 NaCl | - | 1.08 × 10-3 | 6.01 × 10-1 | 6.02 × 10-1 | 12.72 |
Fig. 8. Comparison of specimens surfaces before and after immersion tests.
Fig. 9. (a, c) Plots of OCP vs time and (b, d) polarization curves in 3.38 wt.% NaCl solution at (a, b) pH 7 and (c, d) pH 11.
Fig. 10. SEM micrographs of corroded surface of W80Cu20 in 3.38 wt.% NaCl solution at (a) pH 7 and (b) pH 11 after polarization test; SEM micrographs of corroded surface of W80Cu20 in water at (c) pH 7 and (d) pH 11 after polarization test; and (e) SEM micrograph of W80Cu20 after OCP measurement in 3.38 wt.% NaCl solution at pH 11.
Fig. 11. (a, b) SEM micrographs and (c-e) Elemental mapping of cp Cu and (f) cp W immersed in 3.38 wt.% NaCl solution at pH 7 immersed for 31 days.
Fig. 12. SEM micrographs of W80Cu20 in 3.38 wt.% NaCl solution at pH 7 immersed for (a) 1 day, (b) 13 days and (c) 31 days with (e) XRD patterns, as compared with the corroded morphology of W90Cu10 (d) after 31 days; (f) corrosion rate vs immersion time of cp Cu, cp W, W80Cu20 and W90Cu10 in 3.38 wt.% NaCl solution at pH 7.
Fig. 13. SEM micrographs of W80Cu20 in 3.38 wt.% NaCl solution at pH 11 after immersed for (a) 13 and (c) 31 days with BSE micrographs (b, d).
Fig. 14. SEM micrographs of W80Cu20 in 3.38 wt.% NaCl solution at pH 11 immersed for (a) 1 day and (b) 31 days with (c) XRD pattern; (d) corrosion rate vs immersion time of cp Cu, W80Cu20 and W90Cu10 in 3.38 wt.% NaCl solution at pH 11.
Fig. 15. (a) Plots of OCP vs time and (b) polarization curves in 3.38 wt.% NaCl solution at pH 13; (c) polarization curves in water at pH13.
Fig. 16. Photographs of W80Cu20 during polarization test in 3.38 wt.% NaCl solution at pH 13: (a) cathodic region; (b-e) anodic regions with increasing applied potential; (f) photographs of W80Cu20 surface after test (rinsed by DI water).
Fig. 17. SEM micrographs of W80Cu20 corroded surface in (a) 3.38 wt.% NaCl solution at pH 13 (Fig. 16(f)) and (b) water at pH 13 (without NaCl) after polarization test; and the elemental mapping (c-g) of corroded surface of W80Cu20 in 3.38 wt.% NaCl solution at pH 13 after polarization test.
Fig. 18. SEM micrographs of (a) cp Cu and (b) cp W in 3.38 wt.% NaCl solution at pH 13 after 31 days immersion test; SEM micrographs of W80Cu20 in 3.38 wt.% NaCl solution at pH13 immersed for (c) 3 days, (d) 13 days and (e) 31 days with (f) XRD pattern; and (g) corrosion rate vs immersion time of immersion test of cp Cu, cp W, W80Cu20 and W90Cu10 in 3.38 wt.% NaCl solution at pH 13.
Fig. 19. (a) OCP vs pH and (b) corrosion rate (calculated from the icorr extracted from polarization curves directly) vs pH in 3.38 wt.% NaCl solutions at various pH.
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