EFFECTS OF STRUCTURE AND INTERNAL STRESSES IN OXIDE FILMS ON CORROSION MECHANISM OF NEW ZIRCONIUM ALLOY

doi:10.11900/0412.1961.2014.00261

Acta Metall Sin

2014, Vol. 50

Issue (12): 1529-1537 DOI: 10.11900/0412.1961.2014.00261

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EFFECTS OF STRUCTURE AND INTERNAL STRESSES IN OXIDE FILMS ON CORROSION MECHANISM OF NEW ZIRCONIUM ALLOY

ZHANG Haixia^1,²(

), LI Zhongkui³, ZHOU Lian³, XU Bingshe^1,², WANG Yongzhen⁴

1 Research Center of Advanced Materials Science and Technology, Taiyuan University of Technology, Taiyuan 030024
2 Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024
3 Northwest Institute for Nonferrous Metal Research, Xi′an 710016
4 College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024

Cite this article:

ZHANG Haixia, LI Zhongkui, ZHOU Lian, XU Bingshe, WANG Yongzhen. EFFECTS OF STRUCTURE AND INTERNAL STRESSES IN OXIDE FILMS ON CORROSION MECHANISM OF NEW ZIRCONIUM ALLOY. Acta Metall Sin, 2014, 50(12): 1529-1537.

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Abstract

The corrosion resistance of new zirconium alloys containing Nb, used as the fuel cladding materials in water-cooled nuclear power reactors, is closely related to the characteristics of the oxide films, including the internal stresses and the crystal structure. However, the relation of the corrosion kinetics to the internal stresses and the crystal structure of the oxide films has not been well understood, also the corrosion mechanism of new zirconium alloys has not been confirmed. Therefore, it is helpful to solve the above problems, furthermore improve the corrosion resistance of new zirconium alloys, to characterize the internal stresses and the crystal structure of the oxide films accurately. The internal stresses and the crystal structure of the oxide films of NZ2 zirconium alloy, corroded in 360 ℃, 18.6 MPa lithiated water and 400 ℃, 10.3 MPa steam, were tested by XRD and Raman spectroscopy, and the microstructure of the oxide films was investigated by SEM. The results of the crystal structure show that tetragonal ZrO₂ (t-ZrO₂) content in the oxide films of NZ2 alloy decreases, monoclinic ZrO₂ (m-ZrO₂) content increases with the prolongation of the corrosion time, t-ZrO₂ transforms into m-ZrO₂. And cubic ZrO₂ (c-ZrO₂) appearsin the oxide films when the thickness of the oxide films reaches 2 mm. Corrosion resistance of NZ2 alloy is improved when the content of t-ZrO₂ in the oxide films increases. The results of the internal stresses and the microstructure of the oxide films indicate that the high compressive stresses exist in the oxide films. At the beginning of the corrosion, the compressive stresses in the oxide films increase with the corrosion time. When the thickness of the oxide films reaches 2 mm, the compressive stresses exceed the critical value and the stresses are released. The stress relaxation leads to the formation of the cracks, which reduces the protection of the oxide films, therefore the corrosion transition occurs. After the transition, the compressive stresses of the oxide films are constantly low. So the corrosion transition is closely related to the relaxation of the compressive stresses. The high compressive stresses and t-ZrO₂ content are corresponding to the good corrosion resistance. Also the stabilization mechanisms of t-ZrO₂ and c-ZrO₂ are explored, finally the corrosion mechanism of new zirconium alloys is established.

Key words: zirconium alloy oxide film internal stress crystal structure corrosion mechanism

ZTFLH:

TG146.4

Fund: Supported by National Natural Science Foundation of China (Nos.51372160 and 51242007), Scientific Research Foundation for Returned Overseas Chinese Scholars of Shanxi Province (No.2011-031), Technology Foundation for Selected Overseas Chinese Scholar of Shanxi Province (No.[2011]762)

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	Haixia ZHANG
	Zhongkui LI
	Lian ZHOU
	Bingshe XU
	Yongzhen WANG

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https://www.ams.org.cn/EN/10.11900/0412.1961.2014.00261 OR https://www.ams.org.cn/EN/Y2014/V50/I12/1529

Fig.1 Plots of d-sin²ψ for NZ2 zirconium alloy corroded in 360 ℃ lithiated water for different times (d—interatomic distance of (hkl) diffracting plane, ψ—incidence angle of X-ray, p—slop of d-sin²ψ plot, σ—internal stress of the oxide film)

Fig.2 Plots of d-sin²ψ for NZ2 zirconium alloy corroded in 400 ℃ steam for different times

Fig.3 Relationship of thicknesses and compressive stresses of NZ2 oxide films obtained in 360 ℃ lithiated water and 400 ℃ steam

Table 1 Parameters of NZ2 alloy corroded in 360 ℃ lithiated water and 400 ℃ steam for different times

Fig.4 SEM images of oxide film of NZ2 alloy corroded in 360 ℃ lithiated water for 3 d

(a) low magnification (b) high magnification

Fig.5 SEM images of oxide film of NZ2 alloy corroded in 360 ℃ lithiated water for 294 d

(a) low magnification (b) high magnification

Fig.6 XRD spectra of the oxide films of NZ2 alloy exposed to 360 ℃ lithiated water for different times (The subscripts T, M, C represent tetragonal, monoclinic, cubic ZrO₂, respectively)

Fig.7 XRD spectra of oxide films of NZ2 alloy exposed to 400 ℃ steam for different times

Fig.8 Relationship of corrosion time and tetragonal ZrO₂ content in the oxide film of NZ2 alloy after exposed to 360 ℃ lithiated water and 400 ℃ steam

Fig.9 Raman spectrum of oxide film of NZ2 alloy exposed to 360 ℃ lithiated water for 14 d (The sign T represents tetragonal ZrO₂)

Table 2 Peak positions, intensities (relative to the most intense 177.6 cm^-1) and shifts of peaks of oxide film of NZ2 alloy exposed in 360 ℃ lithiated water for 14 d

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