Tuning the microstructure for superb corrosion resistance in eutectic high entropy alloy

doi:10.1016/j.jmst.2021.08.069

Abstract

Abstract:

In this work, we demonstrate that the corrosion resistance of the FeCrNiCoNb_0.5 eutectic high entropy alloy (EHEA) can be tuned by controlling the size of its eutectic structure. Through microstructure refinement, the EHEA exhibits a superb corrosion resistance in 1 M NaCl in terms of a very low corrosion current density and an ultra-high transpassviation potential, which outperforms a variety of other HEAs and conventional metals and alloys. At the fundamental level, the microstructure refinement results in a rapid formation of a thick and compact passive film with less Cl^- adsorption on the EHEA, which results in significant enhancement in its corrosion resistance. The outcome of our research provides important insights into the design of corrosion resistant chemically complex alloys.

Key words: Eutectic high entropy alloy, Passivation, Transpassivation potential, Microstructure size

S. Shuang, Q. Yu, X. Gao, Q.F. He, J.Y. Zhang, S.Q. Shi, Y. Yang. Tuning the microstructure for superb corrosion resistance in eutectic high entropy alloy[J]. J. Mater. Sci. Technol., 2022, 109: 197-208.

Figures/Tables 12

Fig. 1 (a)-(e) X-ray diffraction (XRD) results and (f)-(j) the typical SEM pictures of the chemically etched lamellar structure obtained from the as-cast wedge sample and plate samples subjected to various level of thermal annealing. (Note that scale bars are equal to 2 μm in (f)-(j)) (For interpretation of the references to color in this figure, the reader is referred to the web version of this article).

Fig. 2. (a) HRTEM image of the FCC-Laves interface. The FFT image of the selected local areas in the FCC phase which corresponds to the position of (b) point 1, (c) point 2 and (d) point c in (a). (e) Averaged local lattice constant in the FCC phase along the yellow arrow in (a). (f) STEM image of the FCC and Laves phase with the elemental profiles across several interfaces. (Note that scale bars are equal to 10 1 /nm in (b)-(d)) (For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article).

Fig. 3. (a)-(e) Potentiodynamic polarisation curves of our EHEA samples with different thermal history. (f) A comparison of the corrosion current density (Icorr) and transpassivation potential (ET) between EHEAs and other materials in 1 M NaCl solution at room temperature. The corrosion morphologies of (g) the L140 and (h) L1500 sample after polarisation. (Note that scale bars equal 10 μm in (g) and (h)).

Table 1. Corrosion properties of our EHEA samples obtained at room temperature in 1 M NaCl solution.

Samples	E_corr (mV_SCE)	I_corr (A · cm^-2)	E_T (mV_SCE)
L80	-173 ± 75	(2.29 ± 0.12) × 10^-8	993 ± 11
L140	-283 ± 41	(6.96 ± 0.80) × 10^-8	974 ± 15
L250	-299 ± 26	(1.46 ± 0.10) × 10^-7	958 ± 8
L700	-301 ± 29	(1.93 ± 0.39) × 10^-7	631 ± 75
L1500	-310 ± 11	(2.17 ± 0.07) × 10^-7	411 ± 62

Table 2. Summary of the corrosion properties (derived from potentiodynamic polarisation curves) of metals and alloys at room temperature in 1 M NaCl solution.

Metals and alloys	I_corr (nA · cm^-2)	E_corr (mV_SCE)	E_T (mV_SCE)	Refs.
FeCrNiCoNb_0.5-L80	23	-173	993	This study
FeCrNiCoNb_0.5-L140	70	-283	974
FeCrNiCoNb_0.5-L250	146	-299	958
FeCrNiCoNb_0.5-L700	193	-301	631
FeCrNiCoNb_0.5-L1500	217	-310	411
FeCoNi	400	-493	-32	[92]
FeCoNiCr	280	-328	-34	[92]
FeCoNiNb	43,000	-494	-235	[91]
CrFeMn_0.5Ni_0.5	450	-631	-222	[93]
FeCoNiNb_0.5Mo_0.5	33,000	-455	295	[91]
Co_1.5CrFeNi_1.5TiMo_0.1	130	-622	973	[63]
Co_1.5CrFeNi_1.5TiMo_0.5	200	-734	923	[63]
Co_1.5CrFeNi_1.5TiMo_0.8	410	-792	941	[63]
Co_1.5CrFeNi_1.5TiMo₀	570	-684	97	[63]
Al_0.3CrFeMn_0.5Ni_0.5	690	-641	-391	[93]
Al_0.5CrFeMn_0.5Ni_0.5	1020	-741	-361	[93]
Cu_0.5NiAlCoCrFeSi	3160	-770	-490	[64]
304 SS^a	30	-196	346	[37]
202 SS^a	24	-110	439	[94]
316 L SS^a	29	-90	606	[94]
Ion Nitriding 316 L SS^a	232	-654	-6	[95]
E309 DSS^b	279	-243	431	[96]
E2209 DSS^b	918	-266	492	[96]
Carbon steel	4L1500	-651	-^c	[97]
AA2024-T3^d	86	-917	-704	[98]
AA2024-T3^d with LBP^e	38	-907	-676	[99]
AA7075^d	1188	-896	-813	[100]
T240^d	70,000	-712	-618	[101]
Ni-based alloy 22	40	-339	597	[102]
Ni_50.8Ti_49.2	2000	-380	358	[103]
Ti₆₀Cu₁₄Ni₁₂Sn₄Nb₁₀	9500	-409	-182	[104]
Copper^f	18,100	-540	-188	[105]
Nickel^f	71,600	-477	174	[106]

Fig. 4. (a) Nyquist and (b) Bode plots of L140 and L1500 samples exposed to 1 M NaCl solution in the single-cylinder corrosion cell under open circuit potential condition. The inset of (a) shows the equivalent circuit. (c) Resistance and passive film thickness obtained from EIS plots. (d) Calculated thickness of the passive film during the potentiostatic oxide growth for L140 and L1500 samples in 1 M NaCl solution.

Table 3. Equivalent circuit elements values for EIS data corresponding to L140 and L1500 samples in 1 M NaCl solution.

Material	R_s (Ω cm²)	Q₁ 10^-6 (Ω^-1 cm^-2 s^-n)	n₁	R₁ (Ω cm²)	Q₂ 10^-6 (Ω^-1 cm^-2 s^-n)	n₂	R₂ 10⁶ (Ω cm²)	χ² × 10^-3
L140	3.65 (0.8)	7.34 (9.8)	0.99 (0.91)	50.65 (14.4)	9.79 (12.4)	0.82 (0.67)	5.75 (10.4)	1.88
L1500	3.68 (1.1)	16.22 (11.0)	0.98 (2.0)	20.81 (19.0)	19.37 (18.2)	0.84 (1.26)	0.90 (7.07)	1.86

Fig. 5. Topography profiles of (a) L1500 sample and (b) L140 sample. The mapping of electronic work function on the surface of (c) L1500 sample and (d) L140 sample. (e, f) The profile of electronic work function along the dash line in (c, d). (Note that scale bars are equal to 2 μm in (a)-(d)) (For interpretation of the references to color in this figure, the reader is referred to the web version of this article).

Fig. 6. High resolution XPS spectra of the passive films formed on the L140 and L1500 sample after passivation for 3 h at + 250 mVSCE in 1 M NaCl solution at room temperature. (a) Cr 2p; (b) Nb 3d; (c) Fe 2p; (d) Ni 2p; (e) Co 2p; (f) O 1s. (g) The calculated cationic fractions of the metallic elements in the passive film of the L140 and L1500 sample.

Fig. 7. (a) Mott-Schottky plots for the passive film formed on L140 and L1500 samples in 1 M NaCl solution at OCP for 3 h. (b) Flat band potential and donor densities of the passive films formed on L140 and L1500 sample.

Fig. 8. (a) Double-layer capacitance as a function of electrode potential for the passive films formed for 3 h at OCP on HEAs with various grain sizes. (b) The measured difference between Ecorr and PZFC for the L140 and L1500 sample (For interpretation of the references to color in this figure, the reader is referred to the web version of this article).

Fig. 9. (a) The calculated critical potential difference ∆ET a function of surface tension of the metal-electrolyte interface for different passive film thickness. (b) Schematics of the microstructural size effect on the passivation on our EHEA in 1 M NaCl solution at room temperature (For interpretation of the references to color in this figure, the reader is referred to the web version of this article).

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