Oxidation of amorphous alloys

doi:10.1016/j.jmst.2018.02.015

Abstract

Abstract:

Owing to their unique short- or medium-range ordered microstructures and excellent mechanical, physical, and chemical properties, amorphous alloys have attracted significant interest in recent years. For the application of amorphous alloys, clarifying their oxidation processes and mechanisms is necessary since many of the surface-related properties of amorphous alloys largely depend on the surface oxide layer. The aim of this paper is to review the recent research on the thermal oxidation behaviors of amorphous alloys under pure oxygen or air condition. The contents are divided into three categories according to the number of components the research considers, i.e., the oxidation of binary, ternary, and multi-component (>3) amorphous alloys. Each section discusses the thermal stability of the amorphous matrix, oxidation kinetics, and the oxide layer and amorphous substrate, which are strongly affected by internal factors (i.e., alloy elements and microstructure) and external factors (i.e., oxidation temperature, duration, and oxygen partial pressure, etc.). The general features of the oxidation of amorphous alloys - from simple binary to complex multi-component amorphous alloys - will be summarized. This overview of the current scientific understanding on the fundamentals of these materials may provide guidelines for the development of strongly corrosion-resistant amorphous alloys.

Key words: Amorphous alloys, Oxidation, Oxidation kinetics, Microstructure, Surface treatment

Zhiqiang Xu, Yifei Xu, An Zhang, Jiangyong Wang, Zumin Wang. Oxidation of amorphous alloys[J]. J. Mater. Sci. Technol., 2018, 34(11): 1977-2005.

Figures/Tables 53

Table 1 Compositions and structures of amorphous AlxZr1-x (am-AlxZr1-x) films at room temperature [30].

Specimen	Al (at.%)	Zr (at.%)	Hf (at.%)	Structure
Al_0.1Zr_0.9	8.7	90.8	0.5	crystalline
Al_0.2Zr_0.8	18	81.5	0.5	crystalline
Al_0.3Zr_0.7	28.9	70.7	0.4	amorphous
Al_0.4Zr_0.6	40.4	59.3	0.3	amorphous
Al_0.5Zr_0.5	50.2	49.5	0.3	amorphous
Al_0.6Zr_0.4	61.8	38	0.2	amorphous
Al_0.7Zr_0.3	72.8	27	0.2	amorphous
Al_0.8Zr_0.2	82.6	17.3	0.1	amorphous
Al_0.9Zr_0.1	91.3	8.6	0.05	crystalline

Fig. 1. Crystallization temperatures and products of amorphous (am)-AlxZr1-x (x = 0.26, 0.35, 0.51, 0.68, and 0.75), as measured by in situ XRD [29].

Fig. 2. Al-Zr binary phase diagram [29].

Fig. 3. Evolution of oxidation layer thickness with oxidation time for am-Al0.44Zr0.56 at 500 and 560 °C (PO2= 1 bar), as measured by spectroscopic ellipsometry (SE) and cross-sectional TEM. Reprinted with permission from Ref. [28], Copyright 2015, Elsevier.

Fig. 4. (a) Cross-sectional TEM of am-Al0.51Zr0.49 oxidized at 400 °C for 10 h in pure O2 (??.?PO2=1 bar). The am-(Al,Zr)-oxide layer formed on the alloy is shown in (b), with the corresponding EELS elemental maps of (c) Zr, (d) O, and (e) Al, and (f) a combined image of the Zr, O, and Al maps. Reprinted with permission from Ref. [24], Copyright 2015, Elsevier.

Fig. 5. Al/Zr ratios of am-AlxZr1-x alloys over a wide composition range before and after oxidation at different temperatures in pure O2 (??.?PO2=1 bar). Both the Al/Zr ratios of the formed am-(Al,Zr)-oxide and the am-AlxZr1-x substrate (after isothermal oxidation) were measured by AES. Reprinted with permission from Ref. [24], Copyright 2015, Elsevier.

Fig. 7. DSC analyses of am-CuxZr1-x (x = 0.6, 0.618, 0.64, and 0.66) conducted at a heating rate of 20 °C/min under vacuum. The specimens were 0.5 mm-thick strips of am-Cu0.6Zr0.4, am-Cu0.618Zr0.382, and am-Cu0.66Zr0.34, a 2 mm-thick strip of am-Cu0.64Zr0.36 and an ～60 μm-thick splat-quenched specimen of am-Cu0.64Zr0.36. Reprinted with permission from Ref. [23], Copyright 2004, Elsevier.

Table 2 Thicknesses (μm) of oxide layers formed on am-Cu0.5Zr0.5, measured by cross-sectional SEM [31].

Oxidation time (h)	350 °C	375 °C	400 °C	425 °C
36	1.81 ± 0.10	2.18 ± 0.08	-	-
100	2.80 ± 0.10	3.48 ± 0.31	-	-
168	3.35 ± 0.08	4.67 ± 0.19	6.00 ± 0.12	7.24 ± 0.21

Table 3 Oxidation rate constants (ks, cm2/s) of am-Cu0.5Zr0.5, pure Cu, and pure Zr in air [31].

Specimen	350 °C	375 °C	400 °C	425 °C
am-Cu_0.5Zr_0.5	2.07 × 10^-13	3.53 × 10^-13	5.69 × 10^-13	9.10 × 10^-13
Pure Cu	-	-	1.16 × 10^-11	3.37 × 10^-11
Pure Zr	-	-	7.31 × 10^-14	3.59 × 10^-13

Fig. 10. (a) Cross-sectional TEM image of am-Zr0.7Cu0.3 after continuous heating to 350 °C, and (b) a HR-TEM image of the region denoted in (a). Reprinted with permission from Ref. [33], Copyright 2014, American Institute of Physics.

Fig. 11. (a) Cross-sectional annular bright-field STEM image, (b) bright-field TEM image of am-Zr0.7Cu0.3 after continuous heating to 400 °C (The inset in (a) gives the XRD analysis), (c) AES sputter-depth profile and (d) HR-TEM image of the area denoted in (b). Reprinted with permission from Ref. [33], Copyright 2014, American Institute of Physics.

Fig. 13. (a) XRD analyses of NixNb1-x (x=0.595, 0.605, 0.61, 0.615, 0.62, and 0.625) rods with a diameter of 2 mm and (b) DSC measurement of am-Ni0.62Nb0.38 performed at a heating rate of 20 °C/min (The melting process is given in the inset). Reprinted with permission from Ref. [20], Copyright 2006, American Institute of Physics.

Fig. 16. (a) Bright-field and (b) dark-field TEM images of am-Ni0.62Nb0.38 oxidized in air at 400 °C for 2 h and (c) size distribution of the Ni particles precipitated in the amorphous Nb2O5 oxide. Reprinted with permission from Ref. [42], Copyright 2013, Elsevier.

Fig. 18. XPS measurements of am-Ni0.65Nb0.35 (a) polished and Ar+-bombarded under vacuum for 12 min, and (b) after oxidation in air at room temperature and (c) in O2 at 400 °C for 30 min. Reprinted with permission from Ref. [43], Copyright 1999, Elsevier.

Fig. 20. Oxidation kinetics of (a) Zr0.7Pd0.3 melt-spun at 10 and 20 m/s and (b) Zr0.8Pt0.2 melt-spun at 10, 20, 30, and 40 m/s. The Zr0.7Pd0.3 and Zr0.8Pt0.2 specimens were continuously heated to 700 °C in a thermal analyzer at a heating rate of 10 °C/min. Reprinted with permission from Ref. [27], Copyright 2008, Elsevier.

Fig. 23. SEM morphologies of (a) am-Zr0.7Pd0.3 (melt-spun at 20 m/s), (b) am-Zr0.7Pd0.3 (10 m/s), and (c) am-Zr0.8Pd0.2 (40 m/s) after continuous heating to 500 °C in air. Reprinted with permission from Ref. [27], Copyright 2008, Elsevier.

Table 4 Tg and Tx values of Cu27.5Zr65.0Al7.5, Cu43Zr50Al7, and Cu47.5Zr47.5Al5 BMGs, measured by DSC at a heating rate of 10 °C/min [[49], [50],52].

BMG	T_g (°C)	T_x (°C)
Cu_27.5Zr_65.0Al_7.5	365	435
Cu₄₃Zr₅₀Al₇	416.2	480.4
Cu_47.5Zr_47.5Al₅	424.3	474.5

Table 5 Kp values (g2 cm-4 s-1) of Cu47.5Zr47.5Al5 BMG and its crystalline counterpart treated at 400-500 °C in air [49].

Alloy	400 °C	450 °C	500 °C
Cu_47.5Zr_47.5Al₅ BMG	4.71 × 10^-12	2.89 × 10^-11	1.06 × 10^-12
Crystalline Cu_47.5Zr_47.5Al₅	5.81 × 10^-13	1.56 × 10^-12	1.80 × 10^-12

Fig. 25. (a) XRD analyses of melt-spun Cu27.5Zr65.0Al7.5 BMG and its specimens annealed at 480 and 780 °C for 1000 s. Oxidation kinetics of the melt-spun and annealed Cu27.5Zr65.0Al7.5 BMG in air at (b) 350 °C and (c) 390 °C. Reprinted with permission from Ref. [52], Copyright 2006, Elsevier.

Fig. 26. Cross-sectional SEM images and corresponding XRD analyses of Cu47.5Zr47.5Al5 BMG oxidized for 36 h at (a) 400 °C and (b) 500 °C. Reprinted with permission from Ref. [49], Copyright 2008, Springer.

Fig. 27. (a) Cross-sectional TEM image of Cu45Zr45Al8Be2 BMG continuously heated to 480 °C in air with a flow rate of 20 cm3/min and (b) a HR-TEM image of the region denoted in (a). Reprinted with permission from Ref. [51], Copyright 2013, Elsevier.

Table 6 ΔG°f (kJ/mol O2) values of oxides of Zr, Cu, Al, and Ti at different temperatures [49].

Material	400 °C	425 °C	450 °C	475 °C	500 °C
ZrO₂	-968.35	-963.69	-959.02	-954.38	-949.73
CuO	-188.87	-184.52	-180.17	-175.82	-171.46
Cu₂O	-238.97	-234.51	-230.06	-225.65	-221.14
Al₂O₃	-976.32	-971.12	-965.91	-960.72	-955.53
TiO	-952.32	-947.96	-943.59	-939.22	-939.22
TiO₂	-820.80	-816.32	-811.83	-807.35	-807.35

Fig. 28. Oxidation kinetics of (a) as-cast Cu60Zr30Ti10 BMG and (b) crystallized Cu60Zr30Ti10 BMG in O2 at different temperatures. Reprinted with permission from Ref. [66], Copyright 2005, Materials Research Society.

Fig. 30. (a) XRD analyses of as-cast Cu60Zr30Ti10 BMG (CZT) and annealed Cu60Zr30Ti10 BMG (CZTA) oxidized at 300-500 °C for 10 h in O2 with a flow rate of 500 cm3/min and (b) XPS sputter-depth profiles of as-cast Cu60Zr30Ti10 BMG oxidized at 300 °C for 10 h. Reprinted with permission from Ref. [66], Copyright 2005, Materials Research Society.

Fig. 31. Oxidation processes of Cu60Zr30Ti10 BMG at 320 °C in air, during which a multi-layered structure forms. Nucleation of the oxidation process begins with the formation of the outer Cu2O layer, and is followed by the formation of an inner (Zr,Ti)O2 and metallic Cu layer. Reprinted with permission from Ref. [65], Copyright 2007, Elsevier.

Table 7 Tg and Tx values of Zr53Ni23.5Al23.5 BMG, measured by DSC at different heating rates [73].

Heating rate (°C/min)	T_g (°C)	T_x (°C)
10	-	528.5
20	513.3	542.3
30	519.5	549.1
40	524.2	553.6
100	534.1	566.2

Fig. 33. Oxidation kinetics of Zr60Ni25Al15 BMG oxidized at (a) 310-350 °C and (b) 370-410 °C in O2 with a flow rate of 100 cm3/min. Reprinted with permission from Ref. [75], Copyright 1996, Materials Research Society.

Fig. 34. Cross-sectional SEM images and corresponding XRD analyses of Zr53Ni23.5Al23.5 BMG oxidized in air for 36 h at (a) 500 °C and (b) 550 °C. Reprinted with permission from Ref. [73], Copyright 2007, Elsevier.

Fig. 35. Oxidation kinetics of (a) Ni60Nb35Sn5 BMG in air at 530-590 °C and (b) Ni62Nb38 and Ni59.35Nb34.45Sn6.2 BMGs in 1 bar O2 at 558 °C. Reprinted with permission from Ref. [[44], [76]], Copyright 2007 and 2016, Elsevier.

Table 8 Kp values (g2 cm-4 s-1) of Zr-based BMGs with different compositions oxidized in air at 300-550 °C, along with their Tg and Tx values [[55], [64],70,79,80].

BMG	Temperature region	T (°C)	K_p (g² cm^-4 s^-1)	Ref.
Zr_46.75Ti_8.25Cu_7.5Ni₁₀Be₂₇	amorphous state	315	2.25 × 10^-16	[79]
	amorphous state	330	9.00 × 10^-16
	T_g	340	-
	supercooled liquid state	345	2.50 × 10^-15
	supercooled liquid state	360	3.72 × 10^-15
(Zr₄₈Cu₃₂Al₈Ag₈Ta₄)_99.25Si_0.75	T_g	423	-	[80]
	supercooled liquid state	430	6.55 × 10^-16
	supercooled liquid state	480	1.59 × 10^-14
	T_x	497	-
	crystallization state	520	4.45 × 10^-14
	crystallization state	560	7.08 × 10^-14
Zr₅₃Cu₂₀Ni₁₂Al₁₀Ti₅	amorphous state	300	linear	[70]
		350	linear
		375	4.82 × 10^-11
	T_g	384	-
	supercooled liquid state	400	6.61 × 10^-11
	supercooled liquid state	425	1.54 × 10^-10
	T_x	441	-
	crystallization state	450	1.44 × 10^-10
	crystallization state	500	4.80 × 10^-12
Zr₅₅Cu₃₀Al₁₀Ni₅	amorphous state	300	linear	[[55], [70]]
		350	1.16 × 10^-11
		375	2.06 × 10^-11
	T_g	400	8.76 × 10^-12
	supercooled liquid state	425	3.65 × 10^-12
	supercooled liquid state	450	8.08 × 10^-13
	T_x	480	-
	crystallization state	500	4.21 × 10^-13
Zr₅₈Cu₂₂Al₁₂Fe₈	amorphous state	350	2.62 × 10^-12	[64]
		375	7.67 × 10^-12
		400	2.84 × 10^-11
	T_g	413	-
	supercooled liquid state	450	2.32 × 10^-11
	T_x	475
	crystallization state	500	1.71 × 10^-11
	crystallization state	550	2.69 × 10^-11
Zr₆₅Cu₁₅Al₁₀Ni₁₀	amorphous state	300	linear	[[55], [70]]
	amorphous state	350	1.05 × 10^-11
	T_g	368	-
	supercooled liquid state	375	1.39 × 10^-12
		400	2.62 × 10^-12
		425	2.02 × 10^-12
	T_x	443	-
	crystallization state	450	1.59 × 10^-12

Fig. 38. Cross-sectional SEM images and corresponding XRD analyses of (Zr48Cu32Al8Ag8Ta4)99.25Si0.75 BMG oxidized in air at (a) 430 °C and (b) 480 °C for 100 h. The inset images in (a) and (b) are the corresponding EDS line profiles of the denoted areas. Reprinted with permission from Ref. [80], Copyright 2014, Elsevier.

Fig. 39. Oxidation kinetics of (Cu0.6Zr0.2Ti0.1)98Y2, Cu60Zr30Ti10, and Cu60Zr20Hf10Ti10 BMGs in air at 300-500 °C. Reprinted with permission from Ref. [67], Copyright 2005, Materials Research Society.

Table 9 Kp values (g2 cm-4 s-1) of Cu-based BMGs with different compositions after oxidation in air at 330-500 °C [[49], [6]3,86,87].

BMG	T (°C)	K_p (g² cm^-4 s^-1)	Reference
Cu₄₂Zr₄₂Al₈Ag₈	330	3.98 × 10^-13	[87]
	370	2.13 × 10^-12
	390	5.71 × 10^-12
	420	3.13 × 10^-12
	450	4.37 × 10^-12
	460	1.66 × 10^-11
Cu₄₃Zr₄₃Al₇Ag₇	375	1.17 × 10^-12	[63]
	400	2.22 × 10^-12
	425	2.50 × 10^-12
	450	5.38 × 10^-12
	500	4.00 × 10^-12
(Cu₄₃Zr₄₃Al₇Ag₇)_99.5Si_0.5	375	1.08 × 10^-12	[63]
	400	1.85 × 10^-12
	425	2.16 × 10^-12
	450	3.13 × 10^-12
	500	2.04 × 10^-12
Cu₄₅Zr₄₅Al₅Ag₅	375	1.49 × 10^-12	[63,86]
	400	2.56 × 10^-12
	425	3.65 × 10^-12
	450	3.82 × 10^-12
	500	1.12 × 10^-12
Cu₄₇Ti₃₄Zr₁₁Ni₈	400	1.36 × 10^-13	[49]
	425	4.60 × 10^-13
	450	9.19 × 10^-12
	475	2.71 × 10^-11
	500	7.79 × 10^-11
Pure Cu	400	2.62 × 10^-12	[49]
	450	1.01 × 10^-11
	500	3.74 × 10^-11

Fig. 40. Cross-sectional TEM images and corresponding XRD analyses of Cu43Zr43Al7Ag7 BMG after oxidation in air at (a) 450 °C and (b) 500 °C for 36 h. Reprinted with permission from Ref. [63], Copyright 2010, Elsevier.

Table 10. Kp values (g2 cm-4 s-1) of Fe48Cr15C15Mo14B6Er2 BMG [91] and [(Fe50Co50)75B20Si5]96Nb4 BMG [92] oxidized in air at 600-725 °C.

BMG	T (°C)	K_p (g² cm^-4 s^-1)	Reference
Fe₄₈Cr₁₅C₁₅Mo₁₄B₆Er₂	600	1.27 × 10^-18	[91]
	625	7.74 × 10^-16
	650	8.68 × 10^-14
	675	1.73 × 10^-9
	700	2.55 × 10^-9
	725	7.12 × 10^-9
[(Fe₅₀Co₅₀)₇₅B₂₀S_i5]₉₆Nb₄	500	2.25 × 10^-14	[92]
	550	1.06 × 10^-12
	600	1.93 × 10^-12
	650	4.12 × 10^-12

Table 11. Kp values of Ti50Cu28Ni15Sn7 BMG at 400-500 °C and Pd43Cu27Ni10P20 BMG at 250-350 °C in air [[56], [57]].

BMG	T (°C)	K_p	Reference
Ti₅₀Cu₂₈Ni₁₅Sn₇	400	4.27 × 10^-7 μm² s^-1	[56]
	450	2.50 × 10^-6 μm² s^-1
	500	1.60 × 10^-5 μm² s^-1
Pd₄₃Cu₂₇Ni₁₀P₂₀	250	4.80 × 10^-16 g² cm^-4 s^-1	[57]
	275	3.70 × 10^-15 g² cm^-4 s^-1
	300	8.60 × 10^-14 g² cm^-4 s^-1
	325	1.10 × 10^-13 g² cm^-4 s^-1
	350	3.20 × 10 ^-13 g² cm^-4 s^-1

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