Please wait a minute...
Shopping Cart Email List Chinese
Advanced Search Fig/Tab
Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

Postal Subscription Code 80-969

2018 Impact Factor: 2.809

Featured Articles  |  Most Downloaded  |  Most Reading
Online Submission Subscribe to Our RSS Content Feed
Front Chem Sci Eng    2013, Vol. 7 Issue (1) : 65-71    https://doi.org/10.1007/s11705-013-1314-9
RESEARCH ARTICLE
Evaluation of precipitation behavior of zirconium molybdate hydrate
Liang ZHANG1(), Masayuki TAKEUCHI2, Tsutomu KOIZUMI2, Izumi HIRASAWA1
1. Graduate School of Applied Chemistry, Faculty of Science and Engineering, Waseda University, Tokyo 169-8555, Japan; 2. Japan Atomic Energy Agency, Ibaraki 319–1194, Japan
 Download: PDF(479 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

In the dissolution step of spent nuclear fuel, there is a world-concern problem that zirconium molybdate hydrate precipitates as a byproduct, and accumulates in some reprocessing equipments. In order to prevent this accumulation, we have developed a new method based on the controlled reaction crystallization of zirconium molybdate hydrate (ZMH) in the reprocessing solution, followed by solid liquid separation. In order to measure the particle size of ZMH, batch crystallization experiments were conducted by varying nitric acid concentration and operating temperature. In result, almost all particle sizes scatter around 1 μm on average, despite the higher concentration of nitric aid and operating temperature, and then small particles grow up as an aggregate sticking to the crystallizer. Moreover, polymorph and color changing were observed by varying the concentration of nitric acid and reaction time. These results suggest that crystal color and adhesiveness are closely related to the particle size of ZMH. And the control of nitric acid concentration and small particle growth would be the useful technique to prevent the ZMH sticking.
Keywords spent nuclear fuel      zirconium molybdate hydrate      cleaning method      accumulation     
Corresponding Author(s): ZHANG Liang,Email:supersyr@fuji.waseda.jp   
Issue Date: 05 March 2013
 Cite this article:   
Liang ZHANG,Masayuki TAKEUCHI,Tsutomu KOIZUMI, et al. Evaluation of precipitation behavior of zirconium molybdate hydrate[J]. Front Chem Sci Eng, 2013, 7(1): 65-71.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-013-1314-9
https://academic.hep.com.cn/fcse/EN/Y2013/V7/I1/65
Fig.1  Experimental apparatus
Fig.1  Experimental apparatus
Concentration of ZrO(NO3)2?2H2O /(mol?L–1)0.05
Concentration of Na2MoO4?2H2O /(mol?L–1)0.1
Concentration of HNO3 /(mol?L–1)3, 5
Reaction time /h2
Reaction temperature /K343–373
Tab.1  Experimental condition
Concentration of ZrO(NO3)2?2H2O /(mol?L–1)0.05
Concentration of Na2MoO4?2H2O /(mol?L–1)0.1
Concentration of HNO3 /(mol?L–1)1, 3
Reaction time /h24
Reaction temperature /K343–363
Tab.2  Experimental condition
Fig.2  ZMH crystals produced in this work
Fig.2  ZMH crystals produced in this work
Fig.3  XRD of ZMH
Fig.3  XRD of ZMH
Fig.4  SEM images of ZMH. Temperatures are varied from 343 K to 373 K and the concentrations of nitric acid are 3 M or 5 M. The length of the bar is 2 μm.
Fig.4  SEM images of ZMH. Temperatures are varied from 343 K to 373 K and the concentrations of nitric acid are 3 M or 5 M. The length of the bar is 2 μm.
Fig.5  Observed white sticking the length of the bar of before crushing is 100 μm, obverse is 5 μm, and verso and lateral side is 2 μm
Fig.5  Observed white sticking the length of the bar of before crushing is 100 μm, obverse is 5 μm, and verso and lateral side is 2 μm
Fig.6  CSD of ZMH. Temperatures are varied from 343 to 373 K and the concentrations of nitric acid are 3 M and 5 M.
Fig.6  CSD of ZMH. Temperatures are varied from 343 to 373 K and the concentrations of nitric acid are 3 M and 5 M.
Fig.7  The solubility of ZMH in nitric acid
Fig.7  The solubility of ZMH in nitric acid
Fig.8  SEM image of ZMH crystal precipitated in 1 M HNO. The length of the bar is 1 μm.
Fig.8  SEM image of ZMH crystal precipitated in 1 M HNO. The length of the bar is 1 μm.
Fig.9  XRD of ZMH crystal precipitated in 1 M HNO
Fig.9  XRD of ZMH crystal precipitated in 1 M HNO
Fig.10  Images of ZMH crystals precipitated in 3 M HNO. The reaction time was (a) 60 min and (b) 120 min
Fig.10  Images of ZMH crystals precipitated in 3 M HNO. The reaction time was (a) 60 min and (b) 120 min
Fig.11  CSD of ZMH in 3 M HNO. The reaction time was (a) 60 min and (b) 120 min
Fig.11  CSD of ZMH in 3 M HNO. The reaction time was (a) 60 min and (b) 120 min
1 Kubota M, Fukase T. Formation of precipitate in high-level waste from nuclear fuel reprocessing. Journal of Nuclear Science and Technology , 1980, 17(10): 783–790
doi: 10.1080/18811248.1980.9732654
2 Cansheng L. Study of precipitation behavior of Mo and Zr in nitric acid solution. Journal of Nuclear Radiochemistry , 1992, 14: 24–30
3 Doucet F J, Goddard D T, Taylor C M, Denniss I S, Hutchison S M, Bryan N D. The formation of hydrated zirconium molybdate in simulated spent nuclear fuel reprocessing solutions. Physical Chemistry Chemical Physics , 2002, 4(14): 3491–3499
doi: 10.1039/b201792j
4 Usami T, Tsukada T, Inoue T, Moriya N, Hamada T, Serrano Purroy D, Malmbeck R, Glatz J P. Formation of zirconium molybdate sludge from an irradiated fuel and its dissolution into mixture of nitric acid and hydrogen peroxide. Journal of Nuclear Materials , 2010, 402(2–3): 130–135
doi: 10.1016/j.jnucmat.2010.05.008
5 Magnaldo A, Masson M, Champion R. Magnaldo. Nucleation and crystal growth of zirconium molybdate hydrate in nitric acid. Chemical Engineering Science , 2007, 62(3): 766–774
doi: 10.1016/j.ces.2006.08.076
6 Chater J. Waste not, want not: nuclear reprocessing and stainless steel. Stainl Steel Wold JST , 2005, 17: 42–47
7 Recktenwarld G D, Deinert M R. Cost probability analysis of reprocessing spent nuclear fuel in the US. Energy Econ JST , 2012, 34(6): 1873–1881
doi: 10.1016/j.eneco.2012.07.016
8 Baja B, Varga K, Szabó N A, Németh Z, Kádár P, Oravetz D, Homonnay Z, Kuzmann E, Schunk J, Patek G. Long-term trends in the corrosion state and surface properties of the stainless steel tubes of steam generators decontaminated chemically in VVER-type nuclear reactors. Corrosion Science , 2009, 51(12): 2831–2839
doi: 10.1016/j.corsci.2009.08.007
9 Matsumura K, Kawamura W, Miyake T. JP Patent, 2000-56077 (2000.02.25)
Viewed
Full text


Abstract

Cited
  Shared   
  Discussed