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Initial dissolution rate of a Japanese simulated high-level waste glass P0798 as a function of pH and temperature measured by using micro-channel flow-through test method

マイクロチャンネル流水試験による模擬高レベルガラス固化体P0798の初期溶解速度のpH,温度依存性測定評価

稲垣 八穂広*; 牧垣 光; 出光 一哉*; 有馬 立身*; 三ツ井 誠一郎 ; 野下 健司*

Inagaki, Yaohiro*; Makigaki, Hikaru; Idemitsu, Kazuya*; Arima, Tatsumi*; Mitsui, Seiichiro; Noshita, Kenji*

マイクロチャンネル流水溶解試験法(MCFT法)を用いて、模擬ガラス固化体の初期溶解速度($$r$$$$_{0}$$)のpH依存性,温度依存性を評価した。その結果、25$$^{circ}$$Cにおいてはシングルパスフロースルー法(SPFT法)などによる既往の結果と同様にV字型のpH依存性を示すことがわかった。しかしながら、70, 90$$^{circ}$$CにおいてはpHが中性の条件で$$r$$$$_{0}$$が一定となるU字型のpH依存性を示し、SPFT法等と異なる結果となった。また、90$$^{circ}$$Cにおいては、pHが8から11の範囲でSPFT法と較べて$$r$$$$_{0}$$が大きく、pH依存性の傾きも大きいことがわかった。温度依存性についてはどのpHにおいてもアレニウス則に従うが、pHの増加に伴ってみかけの活性化エネルギーが増加するという結果となり、溶解メカニズムがpHによって変化することが示唆された。

Dissolution tests were performed for a simulated HLW glass by using a Micro-Channel Flow-Through (MCFT) test to evaluate the initial dissolution rate, $$r$$$$_{0}$$, as a function of pH and temperature. The results indicated that the $$r$$$$_{0}$$ shows a "V-shaped" pH dependence at 25$$^{circ}$$C, which is almost consistent with the previous results measured by using other test methods including Single Pass Flow-Through (SPFT) test. At elevated temperatures, however, the $$r$$$$_{0}$$ shows a "U-shaped" pH dependence with a flat bottom at neutral pH, which differs from the previous results. The results also indicated that the MCFT provided a higher value of the $$r$$$$_{0}$$with a steep slope of pH dependence than the SPFT results at basic pH from 8 to 11 at 90$$^{circ}$$C. With respect to the temperature dependence, the $$r$$$$_{0}$$ increases with temperature according to an Arrhenius law at any pH, and the apparent activation energy increases with pH, which suggests that the dissolution mechanism can change depending on pH.

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パーセンタイル:79.93

分野:Nuclear Science & Technology

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