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논문 기본 정보

자료유형
학위논문
저자정보

이민우 (충북대학교, 충북대학교 대학원)

지도교수
정상문
발행연도
2017
저작권
충북대학교 논문은 저작권에 의해 보호받습니다.

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이 논문의 연구 히스토리 (2)

초록· 키워드

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Pyro-processing is an electrochemical fuel processing technology for recycling the spent fuel into metal fuel for a nuclear fast reactor. The electrochemical processing for oxide fuel consist of electrochemical reduction, electro-refining, and electro-winning. In the electrochemical reduction process, most of uranium and transuranic elements can be reduced easily. However, the electrochemical reduction of rare-earth oxides is fairly difficult because of their thermodynamic stability and high oxygen affinity. It was already reported that the unreduced rare earth oxides react with UCl3 to form UOx in the electro-refining step, which causes serious problems in the electro-refining cell. In this study, co-reduction of rare earth oxides (Nd2O3, CeO2) and NiO has been investigated to increase the reduction degree of the rare earth oxides in the electrochemical reduction. The crystalline structure and morphology of the products were investigated by an X-ray diffraction (XRD) and a scanning electron microscopy(SEM), respectively. The products composition and reduction degree of rare earth oxide were estimated by an energy dispersive X-ray spectroscopy (EDS) and a thermogravimetric analyzer (TGA). CeO2-Nd2O3-NiO mixture was partially converted into NiNd2O4 during calcination, which can be easily reduced in the electrochemical reduction process. At the beginning of electrolysis, NiO in the mixed oxide started to be reduced into Ni metal in molten LiCl containing 1wt.% of Li2O. And then the reduction of the rare earth oxide (CeO2, Ce2O3, and Nd2O3) in the vicinity of the Ni metal took place to become the rare earth-Ni intermetallic compounds. The final products were identified to be RENi5-type intermetallics such as NdNi5 or CeNi5. According to EDS analysis, the oxygen contents of the reduced CeO2-Nd2O3-NiO mixture were found to be 4100 ppm. High reduction degrees of 99.23 and 98.80% were achieved with the Nd2O3-NiO and CeO2-NiO mixtures, respectively. The results demonstrate that co-reduction of rare earth oxides and NiO is an effective way to increase the reduction degree of rare earth oxides.

목차

Ⅰ. 서론 1
1.1 연구배경 1
1.2 연구목적 3
1.3 이론고찰 4
1.3.1 파이로 프로세싱 4
1.3.2 전해환원 공정 6
1.3.3 희토류 산화물의 전해환원 11
Ⅱ. 실험방법 15
2.1 용융염 전해셀 조립 15
2.2 희토류 산화물을 포함하는 혼합산화물 펠렛 제조 18
2.3 전기화학 분석 19
2.3.1 전위제어 실험 19
2.3.2 순환전압전류법(cyclic voltammetry) 19
2.4 전해환원 실험 및 분석 22
2.4.1 전해환원 실험 22
2.4.2 XRD 분석 22
2.4.3 SEM-EDS 분석 23
2.4.4 TGA 분석 23
Ⅲ. 결과 및 고찰 24
3.1 고온 용융염에서 혼합산화물의 전해환원 거동 24
3.1.1 전위제어 분석 24
3.1.2 순환전압전류법(cyclic voltammetry) 분석 27
3.1.3 희토류금속/전이금속 비율에 따른 영향 32
3.2 전해환원 시간에 따른 반응생성물 분석 34
3.2.1 전해환원 메커니즘 34
3.2.2 SEM-EDS 분석 45
3.2.3 혼합산화물의 금속 전환율 분석 51
3.3 Li2O 존재하지 않는 용융염에서의 전해환원 54
Ⅳ. 결론 56

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