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Effects of oxidation states of Np on polarization curve of stainless steel in boiling 3M-HNO$$_{3}$$

沸騰3M-HNO$$_{3}$$溶液中におけるステンレス鋼の分極曲線に及ぼすNpの酸化状態の影響

加藤 千明; 上野 文義; 山本 正弘; 伴 康俊 ; 内山 軍蔵; 野島 康夫*; 藤根 幸雄*

Kato, Chiaki; Ueno, Fumiyoshi; Yamamoto, Masahiro; Ban, Yasutoshi; Uchiyama, Gunzo; Nojima, Yasuo*; Fujine, Sachio*

再処理プロセス溶液に含まれるネプツニウムイオンは、ステンレス鋼の腐食を加速するアクチノイドの1つである。しかし、沸騰硝酸中に含まれる微量のネプツニウムイオンがステンレス鋼の腐食を加速するメカニズムは不明な点がある。ネプツニウムには、硝酸水溶液でいくつかの原子価状態が存在することから、電気化学試験とスペクトル分析を同時に測定可な小型セルを用いて、ステンレス鋼の分極曲線とネプツニウムイオンの原子価状態を比較した。その結果、Npイオンの存在によりステンレス鋼のカソード反応が活性化された。またNp(V)は沸騰3M硝酸中で容易にNp(VI)となり、腐食反応が生じない限り還元されないことが明らかとなった。ネプツニウム(VI)は沸騰3M-HNO$$_{3}$$で再酸化することで、ステンレス鋼のカソード反応を維持し腐食を加速することが明らかとなった。

Neptunium ion contained as one of the fission products in reprocessing solutions is known as a corrosion accelerator of the stainless steel. But it is not clear why remarkable acceleration of corrosion is caused by a slight amount of the Np ion in boiling nitric acid solution. Neptunium has several oxidation states in nitric acid solution. These changeable oxidation states of Np in nitric acid solution are regarded as the cause. Therefore an evaluation of the electrochemical behaviors on stainless steel in nitric acid solution related to the oxidation state of Np is required in order to understand the corrosion acceleration mechanism. A specially designed electrochemical test cell integrated with optical cell for spectroscopic analysis was used for this purpose. From results of electrochemical tests, cathodic reaction on stainless steel was activated by Np ions. Np(VI) ion made the corrosion potential shift nobler than Np(V) and nobler corrosion potential causes increasing corrosion current and accelerating corrosion of stainless steel in nitric acid solution. Np(V) was easily oxidized to Np(VI) in nitric acid solution and Np(VI) was the stable state in boiling 3M-HNO$$_{3}$$. It was considered that role of Np ions was that of mediator to accelerate corrosion due to activating cathodic reaction and re-oxidizing cycle in boiling 3M-HNO$$_{3}$$.

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