Earticle

본 논문에서는 염소화 반응을 통해 Zircaloy-4 (Zry-4) 피복관으로부터 Zr의 회수 연구를 수행하였다. 피복관의 Zr을 전부 ZrCl4로 전환시키기 위해, Zry-4 피복관을 380도에서 70 cc/min Cl2 + 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, 실험상손실은 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.

The recovery of Zr from Zircaloy-4 (Zry-4) cladding hulls using a chlorination method was demonstrated for complete conversion of Zr into ZrCl4. A chlorination reaction was performed by reacting Zry-4 hulls for 8 h under a 70 cc/min Cl2 + 70 cc/min Ar flow at 380oC. 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.

우리나라에서의 고준위폐기물 처분을 위한 연구는 1997년부터 시작하였으며, 국내에서 발생하는 경수 로 사용후핵연료와 중수로 사용후핵연료를 처분대상으로 하여 2006년도에는 한국형 사용후핵연료 기준 처분시스템(KRS) 개발을 완료하였다. 이후, 경수로 사용후핵연료로부터 재활용 가능물질을 회수하는 재 순환주기를 고려하여 재활용을 위한 파이로공정 연구를 수행하고 있어, 이 공정으로부터 발생하는 고준 위폐기물에 대한 처분연구를 수행하고 있다. 본 논문에서는 심지층 처분시스템 개념설정에 중요한 인자 인 파이로공정으로부터 발생하는 처분대상 폐기물인 세라믹고화 폐기물과 금속폐기물에 대한 특성분석 결과와 폐기물별로 특성에 적합한 처분용기 개념을 기술하였다. 이를 바탕으로 처분대상 폐기물에서 발 생하는 붕괴열의 특성을 고려한 열해석을 통하여 지하처분시설에서의 처분용기 간격과 처분동굴 간격을 결정하고, 이를 반영하여 심지층 처분 시스템(A-KRS) 개념을 도출하였다. 이렇게 도출된 처분시스템 입지를 검토하기 위하여 KURT 시설 부지를 대상으로 가상부지로 설정하고, 가상 부지에 대한 지질 및 수리 특성을 이용하여 최적의 배치(안)을 제시하였다. 본 연구의 결과는 추후 실제 부지특성자료와 연계하여 처분장 설계 및 처분안전성 평가에 입력자료로 활용될 것이다.

A long-term R&D program for HLW disposal technology development was launched in 1997 in Korea and Korea Reference disposal System(KRS) for spent fuels had been developed. After then, a recycling process for PWR spent fuels to get the reusable material such as uranium or TRU and to reduce the volume of radioactive waste, called Pyro-process, is being developed. This Pyro-process produces several kinds of wastes including metal waste and ceramic waste. In this study, the characteristics of the waste from Pyro-process and the concepts of a disposal container for the wastes were described. Based on these concepts, thermal analyses were carried out to determine a layout of the disposal area of the ceramic wastes which was classified as a high level waste and to develop the disposal system called A-KRS. The location of the final repository for A-KRS is not determined yet, thus to review the potential repository domains, the possible layout in the geological characteristics of KURT facility site was proposed. These results will be used in developing a repository system design and in performing the safety assessment.

Securing the safeguardability of a reprocessing process for spent nuclear fuels (SNFs) is imperative. Particularly, the quantity of special nuclear materials inside SNFs must be estimated with the highest achievable precision. Unlike aqueous reprocessing, pyro-processing involves handling input materials in a solid state. Hence, partially extracted samples analyzed by destructive assay (DA) should maintain an acceptable level of representativeness. In this study, a representative sampling method widely applied in the pharmaceutical industry was adopted for homogenization in the head-end process of pyro-processing. By employing representative sampling, specifically based on the mechanism of the rotary riffler, the overall process of homogenization prior to DA analysis was simplified, and less probable hold-up that could contribute to materials unaccounted for (MUF) would be expected. The resulting Pu sampling uncertainty was confirmed to be less than 1% (for ≥ 1,000 ㎛ particle size and ≤ 5 kg sample mass), ensuring sufficient control of Pu accounting uncertainty at a reasonably low level (≤ 1%). Thus, representative sampling can be a competitive alternative to previously suggested methodologies.

Pyro-process of solids is the way to heat solid materials under high temperature. In this processing, energy efficient use is one of the main concerns due to its high energy consumption of bulk materials. To calculate the energy use of processes, heat & mass balance in simplified 0-dimensional model was performed. Energy calculation by this simplified model can lead to confusion due to simplification. Thus, it is necessary to understand considerations of energy analysis. In this study, cement manufacturing as a very common example of pyro-processing of solids, was introduced for explaining considerations of energy analysis for energy efficient use.