Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT) (방사성폐기물학회지)

Korean Radioactive Waste Society (한국방사성폐기물학회)
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Evaluation of Na2CO3-H2O2 Carbonate Solution Stability

Na2CO3-H2O2 탄산염 용액의 안정성 평가

  • Received : 2011.04.14
  • Accepted : 2011.06.29
  • Published : 2011.09.30
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Abstract

This study was carried out to examine the stability of $Na_2CO_3-H_2O_2$ carbonate solution with aging time in the dissolving solution after oxidative dissolution of U by a carbonate solution, the Cs/Re filtrate after selective precipitation of Cs and Re (as a surrogate for Tc), and the acidification filtrate after precipitation of U by acidification, respectively. The compositions of dissolving solution were not changed with ageing time, and the selective precipitation of Re and Cs was also not affected without regard to the aging time of dissolving solution. The successive removal of Cs and Re from a carbonate dissolving solution was possible. However, the recovery yield of U by acidification was decreased with increasing the aging time of the dissolving solution and the Cs/Re-filtrate, respectively, because U was converted from the uranyl peroxocarbonato complex to the uranyltricarbonate in the solution aged for a long time. Accordingly, it is effective that a dissolving solution and a Cs/Re filtrate are treated within the aging of 7 days, respectively, in order to recover U more than 99%. On the other hand, the recovery of U was carried out in order of the oxidative dissolution of U selective precipitation of Re and Cs precipitation of U by acidification. Almost all of U and a part of FP were co-dissolved in oxidative dissolution step. Over 99% of Re and Cs from the FP co-dissolved with U could be removed by a TPPCl (tetraphenylphosphonium chloride) and a NaTPB (sodium tetraphenylborate), respectively. U was precipitated nearly 100% by acidification to pH 4. Therefore, it was confirmed that the validity of recovery of U by precipitation methods from a SF (spent fuel) in the $Na_2CO_3-H_2O_2$ solution.

연구는 $Na_2CO_3-H_2O_2$ 탄산염 용액의 숙성시간에 따른 안정성을 U의 산화 용해액, Cs/Re의 선택적 침전 여과액 및 U의 산성화 침전 여과액으로 구분하여 검토하였다. 숙성시간에 따른 산화 용해액 내 조성 변화는 거의 없었으며, Cs/Re의 선택적 침전에도 아무 영향이 없이 산화 용해액으로부터 순차적으로 Re과 Cs의 침전제거가 가능하였다. 그러나 U의 산성화 침전에서는 산화 용해액이나 Cs/Re의 선택적 침전 여과액을 장시간 동안 숙성시킬 경우 U이 uranyl peroxocarbonato complex에서 uranyltricarbonate로 일부 전환되어 U의 침전회수를 감소시켰다. 그러므로 99% 이상의 U을 회수하기 위해서는 산화 용해액 및 Cs/Re의 선택적 침전 여과액의 숙성시간을 각각 7일 이내에서 처리하는 것이 효과적이다. 그리고 SF 의 산화/용해${\rightarrow}$Cs과 Re(/Tc)의 선택적 침전${\rightarrow}$ U의 산성화 침전 등을 순차적으로 수행하여, 산화/용해에서는 대부분의 U과 FP 중 일부가 함께 용해 되었으며, 함께 용해된 FP 중 Re과 Cs은 각각 TPPCl 및 NaTPB로 99% 이상을 침전제거할 수 있었다. 그리고 산성화 (pH 4) 침전에서는 U을 거의 100% 침전회수 하여 $Na_2CO_3-H_2O_2$ 탄산염 용액에서 침전법으로 SF로부터 U 만의 회수 타당성을 확인하였다.

Keywords

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