핵연료분말 제조공정 여액으로부터 Uranyl-peroxide 화합물의 제조

정경채; 김태준; 최종현; 박진호; 황성태

Journal of the Korean Industrial and Engineering Chemistry, Vol.8, No.3, 430-437, June, 1997

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핵연료분말 제조공정 여액으로부터 Uranyl-peroxide 화합물의 제조

Uranyl Peroxide Compound Preparation from the Filtrate for Nuclear Fuel Powder Production Process

정경채, 김태준, 최종현, 박진호, 황성태

초록

핵연료 분말제조 공정에서 발생하는 여액중의 미량 우라늄과 과산화수소 용액을 반응시켜 uranyl-peroxide 화합물을 제조하였다. 여액에 CO₃^2-가 공존할 경우에는 용해되어 있는 UO₂²⁺가 침전되지 않기 때문에, 여액을 98℃로 가열하여 CO₃^2-를 우선 제거하였다. Uranyl-peroxide 화합물 제조시 최적조건으로는 암모니아 가스로 여액의 pH를 9.5로 조절한 후 과량의 과산화수소 용액을 10ml/lit.-filtrate로 첨가하여 1시간 ageing시킬 때이며, 처리후 여액중의 우라늄농도는 3ppm 이하로 나타났다. 제조된 uranyl-peroxide 화합물을 FT-IR, X-ray, TG 및 화학분석 등을 통해 분석한 결과 화합물의 조성은 UO₄·2NH₄F로 나타났으며, 초기 생성된 1∼2㎛의 UO₄·2NH₄F 입자들은 반응온도 60℃ 및 pH 9.5에서 약 4㎛로 성장하였다. 최적조건에서 제조된 입자들의 고/액 분리효율은 pH의 증가 및 반응온도의 상승에 따라 증가하는 경향으로 나타났다. 한편, 제조된 입자들의 결정형태는 SEM 및 XRD에 의한 분석결과 octahedral 형태로 나타났으며, 이 분말을 공기분위기에서 650℃까지 열분해한 결과 U₃O₈으로 판명되어 핵연료 분말제조 공정으로 재순환이 가능하였다.

Uranyl-peroxide compound was prepared by the reaction of excess hydrogen peroxide solution and trace uranium in filtrate from nuclear fuel conversion plant. The CO₃^2- in filtrate was removed first by heating more than 98℃, because uranyl-peroxide compound could not be precipitated by CO₃^2- remaining in filtrate. The optimum condition for uranyl-peroxide compound was ageing for 1 hr after controling the pH with NH₃ gas and adding the excess H₂O₂ of 10ml/lit.-filtrate. Uranium concentration in the filtrate was appeared to 3 ppm after the precipitation of uranyl-peroxide compound, and the chemical composition of this compound was analyzed to UO₄·2NH₄F with FT-IR, X-ray diffractometry, TG and chemical analysis. Also, this fine particle, about 1∼2㎛, could be grown up to 4 ㎛ at pH 9.5 and 60℃. The separation efficiency of precipitate from mother liquor was increased with increase of pH and reaction temperature. Otherwise, the crystal form of this particle showed octahedral by SEM and XRD, and U₃O₈ powder was obtained by thermal decomposition at 650℃ in air atmosphere.

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[1] Assmann H, Becker M, Trans. Am. Nucl. Soc., 31, 147 (1979)

[2] Brandau E, Dorr W, Trans. Am. Nucl. Soc., 31, 148 (1979)

[3] Jancic SJ, Grootscholton PAM, "Industrial Crystallization," Delft University Press, Boston (1986)

[4] Nyvlt J, "Industrial Crystallization from Solution," CRC Press, Butterworth & Co Ltd. (1971)

[5] Mullin JW, "Crystallization," 3rd ed., Butterworth-Heinemann, Oxford (1971)

[6] Jeong KC, Hwang ST, J. Korean Ind. Eng. Chem., 8(1), 99 (1997)

[7] 장인순, "AUC 제조 및 그의 액체 폐기물 처리에 관한 연구, UF₆의 재전환 단위 공정의 화학특성 연구," 한국에너지연구소, KAERI/RR-240/80 (1980)

[8] 박진호, "재변환공정 부산물인 NH₄F의 재사용 가능성에 관한 연구," 한국원자력연구소 (1992)

[9] Chernayaev II, "Complex Compounds of Uranium," Israel Program for Scientific Translations, Jerusalem (1966)

[10] Dokuzoguz H, Muller HM, Environ. Sci. Technol., 8, 1014 (1974)

[11] Chia L, Ricketts S, "Basic Techniques and Experiments in Infrared and FT-IR Spectroscopy," PERKIN ELMER (1988)

[12] Nakamoto K, "Infrared and Raman Spectra of Inorganic and Coodination Compounds," 3rd ed., John Wiley & Sons, New York (1978)

[13] Bachmann HG, J. Inorg. Nucl. Chem., 36, 795 (1974)

[14] Nielsen AE, "Kinetics of Precipitation," International Series of Monographs on Analytical Chemistry, Vol. 18, Pergamon Press, Oxford (1964)

[15] Haelldahl L, Soerensen OT, "Thermal Analysis," ICTA 80 Birkhaeuser, Boston (1980)

[16] Jenkins R, McClune WF, "JCPDS Powder Diffraction File, Inorganic Phases," International Centre for Diffraction Data, Park Lane, PA, USA (1986)

[17] Halldahal L, Nygren M, J. Nucl. Mater., 138, 99 (1986)