Effect of atomic structure on preferential oxidation of alloys: amorphous versus crystalline Cu-Zr

doi:10.1016/j.jmst.2019.10.001

Abstract

Abstract:

The effect of structural order in the parent alloy substrate on the oxidation kinetics and oxide phase evolution was investigated for the thermal oxidation of amorphous Cu_33at.%Zr_67at.% and crystalline CuZr₂ alloys of identical compositions in the temperature range of 200-250 °C. It was found that, besides the strong preferential oxidation of Zr in both alloys, the lack of structural order in the amorphous Cu_33at.%Zr_67at.% alloy results in much slower oxidation kinetics, as well as in distinctly different microstructures of the oxide overgrowth and its Zr-depletion zone in the wake of the ZrO₂ overlayer growth front. The experimental findings can be rationalized on the basis of the strikingly different atomic mobilities of Cu, Zr and dissolved O in the amorphous and crystalline alloys, which also results in different nucleation barriers for crystalline oxide nucleation. The thus obtained knowledge on the underlying oxidation mechanisms provides new and profound insights into the surface engineering of metallic alloys.

Key words: Oxidation, Atomic structure, Amorphous alloys, Cu-Zr, HRTEM

Yifei Xu, Lars P.H. Jeurgens, Peter Schützendübe, Shengli Zhu, Yuan Huang, Yongchang Liu, Zumin Wang. Effect of atomic structure on preferential oxidation of alloys: amorphous versus crystalline Cu-Zr[J]. J. Mater. Sci. Technol., 2020, 40: 128-134.

Figures/Tables 7

Table 1 Gibbs energies of formation (ΔGf) at 200-250 °C of corresponding oxide phases (unit: kJ/mol O2). All necessary thermodynamic data were taken from [18].

Oxide phase	ΔG_f (kJ/mol O₂) at
Oxide phase	200 °C	225 °C	250 °C
am-ZrO₂	-943.3	-939.2	-935.0
m-ZrO₂	-1006.1	-1001.4	-996.6
CuO	-224.5	-220.0	-215.5
Cu₂O	-269.1	-265.3	-261.5

Fig. 1. XRD patterns of the as-deposited/as-polished and oxidized (a) am-Cu33at.%Zr67at.% and (b) c- C uZr2 alloys, and (c) OM image of the as-polished c-CuZr2 alloy.

Fig. 2. AES depth-profiles of am-Cu33at.%Zr67at.% alloys oxidized at (a) 200 °C, (b) 225 °C, (c) 250 °C for 10 h and c-CuZr2 alloys oxidized at (d) 200 °C, (e) 225 °C and (f) 250 °C for 10 h.

Table 2 Thicknesses of oxide layers (dox) and Zr-depleted region (dZrdepleted) on the Cu-Zr alloys and concentration of dissolved oxygen in the Cu-Zr alloys (cO).

Specimen	Time	d_ox±0.5 (nm)			d_Zrdepleted±0.5 (nm)			c_O±0.1 (at.%)
Specimen	Time	200 °C	225 °C	250 °C	200 °C	225 °C	250 °C	200 °C	225 °C	250 °C
am- Cu_33at.%Zr_67at.%	1 h	5.2	9.6	11.5	14.8	14.0	15.6	2.8	3.9	4.7
	4 h	7.9	11.9	12.3	16.5	14.1	20.1	3.3	4.5	5.5
	10 h	10.7	12.6	10.9	21.8	25.8	28.4	4.4	4.9	6.9
c-CuZr₂	10 h	13.6	16.8	22.5	19.4	24.5	26.3	5.1	5.5	10.2

Fig. 3. (a) Cross-sectional TEM image of am-Cu33at.%Zr67at.% alloy oxidized at 250 °C for 10 h, (b) HR-TEM and (c) EDX linescan of the surficial region on the oxidized am-Cu33at.%Zr67at.% alloy.

Fig. 4. (a) Cross-sectional TEM image of c-CuZr2 alloy oxidized at 250 °C for 10 h, (b) HR-TEM of the oxide layer region (rectangle in (a)), and (c) the corresponding EDX elemental linescan of the surface oxide region.

Fig. 5. Schematic illustration of structure of thermal oxidized (a) am-Cu33at.%Zr67at.% and (b) c- CuZr2 alloys.

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