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

  • 제11권1호
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  • Pages.69-75
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  • 2013
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  • 1738-1894(pISSN)
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  • 2288-5471(eISSN)
한국방사성폐기물학회 (Korean Radioactive Waste Society)
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Zircaloy-4 피복관의 염소화 반응 거동: 산화 공정이 반응 속도에 미치는 영향에 대한 기초 연구

Chlorination Reaction Behavior of Zircaloy-4 Hulls: A Preliminary Study on the Effect of the Oxidation Process on the Reaction Rate

  • 투고 : 2013.01.07
  • 심사 : 2013.02.13
  • 발행 : 2013.03.30
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초록

본 연구에서는 산화 공정이 Zircaloy-4 (Zry-4) 피복관의 염소화 반응 속도에 미치는 영향을 연구하기 위하여 Zry-4 피복관의 염소화 반응 실험을 수행하였다. 2시간 마다 반응 생성물을 회수하며 총 6 시간 동안 염소화 반응 실험을 수행하였고, 이를 통해 500도에서 10 시간 동안 산화된 Zry-4의 경우 초기 0-2 시간 구간에서 반응 속도가 현저히 저하되는 것을 확인하였다. 반응 잔류물은 fresh Zry-4와 산화된 Zry-4에서 각각 초기무게의 0.95, 1.65wt%로 확인되었다. 회수된 Zr의 순도는 두 경우 모두 99.61wt%로 동일하였다. 반응 속도의 정량적 분석을 위해 피복관의 반응 시간을 0.5, 1, 2, 4 시간인 경우에 대해 실험을 수행하였다. 실험 결과 분석을 통해 fresh Zry-4의 경우 전 영역에 걸쳐 23.35wt%/h의 단위 시간당 무게감소를 확인할 수 있었고, 산화된 Zry-4의 경우 반응 속도가 두 영역으로 나뉘는 것을 확인하였다. 산화된 Zry-4의 무게 감소 속도는 0-20wt% 영역에서는 17.12wt%/h, 20-100wt% 영역에서는 27.16wt%/h으로 나타났다.

The recovery of Zr from Zircaloy-4 (Zry-4) cladding hulls was demonstrated to investigate the effect of the oxidation process on the reaction rate of the chlorination reaction. In chlorination reaction experiments performed for 6 h, where reaction products were collected every 2 h, it was observed that a significant decrease in the reaction rate was caused by the oxidation process ($500^{\circ}C$, 10 h under an air atmosphere) within the reaction period of 0 - 2 h. The amount of reaction residue increased from 0.95 to 1.65wt% of initial weights in the fresh and Zry-500-10 (Zry-4 hulls oxidized at $500^{\circ}C$ for 10 h under an air atmosphere) hulls, respectively. The purity of the recovered Zr was identical at 99.61wt% for the fresh Zry-4 and Zry-500-10 hulls. Quantitative analysis of the chlorination reaction rate was performed by varying the reaction time from 0.5 to 1.0, 2.0, and 4.0 h. The fitting results showed that the relationship between weight loss and reaction time can be interpreted by a linear line with a slope of 23.35wt%/h for the fresh Zry-4 case, while two linear lines were necessary to fit the results of Zry-500-10. In addition, the slope values were 17.12 and 27.16wt%/h for (0 - 20) and (20 - 100)wt% loss regions, respectively.

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  3. Surface Analysis Study on ZIRLO Cladding Hulls Oxidized at Low Temperatures vol.12, pp.3, 2014, https://doi.org/10.7733/jnfcwt.2014.12.3.235
  4. A TGA study on the chlorination reaction kinetics of Zircaloy-4 cladding hulls vol.459, 2015, https://doi.org/10.1016/j.jnucmat.2015.01.034
  5. Zirconium tetrachloride revisited vol.74, pp.3, 2018, https://doi.org/10.1107/s205322961800219x