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

Korean Radioactive Waste Society (한국방사성폐기물학회)
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Demonstration of Zr Recovery from 50 g Scale Zircaloy-4 Cladding Hulls using a Chlorination Method

50 g 규모의 Zircaloy-4 피복관으로부터 염소화 방법을 이용한 Zr 회수 거동 연구

  • Received : 2012.12.04
  • Accepted : 2013.01.30
  • Published : 2013.03.30
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Abstract

The recovery of Zr from Zircaloy-4 (Zry-4) cladding hulls using a chlorination method was demonstrated for complete conversion of Zr into $ZrCl_4$. A chlorination reaction was performed by reacting Zry-4 hulls for 8 h under a 70 cc/min $Cl_2$ + 70 cc/min Ar flow at $380^{\circ}C$. The initial weight of the reactant (51.7 g) decreased to 0.49 g after 8 h of operation, which is only 0.95wt% of the initial weight. The weight of the total reaction products was 121.7 g with a high Zr purity of 99.80wt%. Fe and Sn were identified as major (0.18wt%) and minor (0.02wt%) impurities of the reaction products, respectively. It was also shown that Zr exhibited a high recovery ratio of 96.95wt% with a relatively small experimental loss of 2.34wt%. Observation of the reaction residues revealed that the chlorination reaction was dominant along the longitudinal direction, and surface oxide layers remained as reaction residues. The high purity and recovery ratio of Zr proposed the feasibility of the chlorination technique as an effective hull waste treatment method.

본 논문에서는 염소화 반응을 통해 Zircaloy-4 (Zry-4) 피복관으로부터 Zr의 회수 연구를 수행하였다. 피복관의 Zr을 전부 $ZrCl_4$로 전환시키기 위해, Zry-4 피복관을 380도에서 70 cc/min $Cl_2$ + 70 cc/min Ar 기체를 이용하여 8시간 동안 반응시켰다. 피복관의 초기 무게는 51.7 g이었으나, 8 시간 반응 후에는 0.49 g만이 잔류물로 남아있는 것을 확인하였는데 이는 초기 무게의 0.95wt%에 해당하는 값이다. 반응 생성물의 무게는 121.7 g 이었으며, Zr의 순도는 99.80wt%였다. 주요 불순물로는 Fe (0.18wt%)와 Sn (0.02wt%)를 확인할 수 있었다. 실험 결과를 통해 확인한 Zr의 회수율은 96.95wt%였으며, 실험상 손실은 2.34wt%로 확인되었다. 반응 잔류물의 관찰을 통해 염소화 반응이 길이 방향으로 주로 일어나며, 표면의 산화층이 반응 잔류물로 남는다는 것을 확인할 수 있었다. 본 연구를 통해 확인된 Zr의 높은 순도와 회수율은 염소화 공정이 폐 피복관 처리 방법으로 매우 유망한 기술임을 의미한다고 볼 수 있다.

Keywords

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