Development of Matrix for the Immobilization of High Level Radioactive Waste : Study on the Synthesis of Ce-pyrochlore

고준위 핵페기물의 고정화를 위한 메트릭스 개발 : Ce파이로클로어 합성 연구

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  • Yudintsev, S. V²
  • Published : 2002.02.01

Abstract

Ce-pyrochlore (CaCe $Ti_2 $O_7)was synthesized to study its properties and phase relations in CaO-Ce $O_2$-Ti $O_2$ system because Ce-pyrochlore was known as a promising material for the immobilization of radioactive actinide. The samples were prepared from the high purity starling materials under the pressure of 200~400 kg/$\textrm{cm}^2$ at room temperature, and annealed at 1000~ 150$0^{\circ}C$. The Synthesized samples were analysed and indentified with XRD and SEM/EDS methods. The optimal formation condition of Ce-pyrochlore was at 130$0^{\circ}C$ under $O_2$ atmosphere and the chemical composition of it wasCa$Ca_{1-x}Ti_{2-y}O_{7-x-2y}$(x=0.03-0.05, y=0.02~0.04) At temperature between 130$0^{\circ}C$ 140$0^{\circ}C$, Ce-pyrochlore underwent rapidly the incongruent decomposition to perovskite. Ce-perovskite, a partial solid solution between perovskite and loparite (C $e_{0.66}$Ti $O_3$), was observed as a major phase above 140$0^{\circ}C$.>.

Ce-파이로클로어(Ce-pyrochlore; CaCe $Ti_2 $O_7)는 장주기 방사성 폐기물인 악티나이드 원소들을 고정화시킬 수 있는 새로운 물질이므로 Ce-파이로클로어를 합성하여 강평형 관계 및 특성을 연구하였다. 혼합된 시료는 상온에서 200-400kg/$\textrm{cm}^2$의 압력으로 성형한 후, 1000-150$0^{\circ}C$ 범위에서 소결온도 및 분위기를 변화시키면서 소성하였다. 합성된 시료는 XRD, SEM/EDS를 사용하여 상분석과 정량분석을 실시하였다. 실험결과, Ce-파이로클로어이 최적 합성조건은 산소분위기 하에서, 130$0^{\circ}C$로 소결하였을 때였으며, 이때의 화학조성은 $Ca_{1-x}Ti_{2-y}O_{7-x-2y}$ (x=0.03-0.05, y=0.02~0.04) 으로써 비화학양론적인 특성을 보였다. Ce-파이로클로어는 1300~140$0^{\circ}C$에서 빠른 비조화 분해현상을 나타내었으며, 140$0^{\circ}C$ 이상에서는 페로브스카이트(perovskite)와 로파라이트(loparite; $Ce_{0.66}TiO_{3}$)사이의 부분 고용체인 Ce(III)페로브스카이트가 주요상으로써 관찰되었다.

Keywords

References

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