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Time dependence of corrosion behavior on Ta in NaOH solutions

TaのNaOH水溶液中における腐食挙動の時間依存性

石島 暖大 ; 上野 文義  ; 阿部 仁 

Ishijima, Yasuhiro; Ueno, Fumiyoshi; Abe, Hitoshi

核燃料再処理機器に使用されているタンタルについて、除染作業での使用が想定される水酸化ナトリウム溶液における腐食挙動の時間依存性を浸漬腐食試験により調査し、経時変化の機構について表面観察および電気化学測定結果から検討した。浸漬腐食試験についてNaOH濃度は1から7mol/L、浸漬時間はそれぞれ、24から168hrとし、室温で行った。腐食速度はNaOH濃度とともに増加するが、浸漬時間によりピークを示しその後減少した。ピークまでの時間はNaOH濃度が高いほど短時間であった。浸漬腐食試験後に洗浄・秤量を行った試料表面のSEMおよびラマン分析では皮膜の生成はみられなかった。一方、分極抵抗は浸漬直後から減少した後に一定値あるいは増加を示した。分極抵抗の経時変化は腐食速度の変化と同じ挙動を示し、また分極抵抗の値は皮膜抵抗と電荷移動抵抗の和とおおよそ一致することから、腐食速度の経時変化は浸漬による皮膜生成に影響を受けることが示唆された。皮膜は主としてTaの溶解により生成するNa$$_{8}$$Ta$$_{6}$$O$$_{19}$$であると考えられた。

The time dependence of the corrosion behavior of tantalum (Ta), which is used in nuclear fuel reprocessing equipment, in sodium hydroxide (NaOH) solutions was investigated by immersion tests, and the mechanism of the time dependence was examined via surface observations and electrochemical measurements. The immersion tests were conducted at room temperature with NaOH concentrations ranging from 1 to 7 mol/L for immersion periods of 24 to 168 h. The corrosion rate increased with the NaOH concentration but peaked with the immersion period and then decreased. The time to peak of the corrosion rate was shorter with higher NaOH concentration. The X-ray diffraction (XRD) patterns and Raman spectra of the surfaces of the specimens immersed in the 7 mol/L NaOH solution for more than 48 h showed Na$$_{8}$$Ta$$_{6}$$O$$_{19}$$ formation. The polarization resistance decreased with immersion time for all NaOH concentrations up to about 24 h after immersion. Thereafter, the polarization resistance increased with immersion time in 7 mol/L NaOH solution and remained almost constant in the other NaOH concentrations. Findings suggested that the change in the corrosion rate was affected by the film formation during immersion, since the time dependence of the polarization resistance and the sum of film resistance and charge transfer resistance had the same tendencies. The precipitation film was mainly Na$$_{8}$$Ta$$_{6}$$O$$_{19}$$ formed by the dissolution of the passivity film on Ta.

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