EG0000334
Third Arab Conference on the Peaceful Uses of Atomic Energy, Damascus 9 -13 Dec. 1996 AAEA Production of Nuclear Grade Uranium Trioxide by a Non-Conventional Method
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Abstract
A non-conventional method to produce nuclear grade uranium trioxide (orange oxide) from crude yellow cake has been proposed. The method depends on selective leaching of uranium from the yellow cake using ammonium carbonate and selective precipitation of uranyl ion from the obtained leach solution using hydrogen peroxide. In carrying out the optimization of the leaching of uranium, it was found that 130 g/L of ammonium carbonate will be required for complete dissolution of uranium from the present yellow cake at a solid/liquid ratio of 1/10, a reaction temperature of 50°C and 6 h mixing time. Nitric acid is added to the leach solution to convert uranyl carbonate solution (pH=8) to uranyl nitrate (pH=2.7). Afterwards, uranium peroxide is precipitated from the uranyl nitrate solution by adding hydrogen peroxide and ammonia solution in presence of 5% (W/V) EDTA solution for masking impurities. Finally, uranium trioxide dihydrate (UO3.2H2O) is obtained by reducing the precipitated uranium peroxide with 2M sodium thiosulphate solution at ambient temperature. Nuclear purity of the product has been confirmed by determination of trace impurities using Inductively Coupled Plasma-Mass spectrometer (ICP-MS) instrument. The proposed flowsheet requires indeed a clean simple technology with relatively cheap equipment and would realize economic savings. *-1 "i\y 4 t) i| a" > i^-o (nuclear grade UO3)) 3. JJ I o ^Ij ot_i la">ll ILj Ul j (crude yellow cake) C3^e) <= l^i. . (solvent extraction) ~<-*j-^ *JI CJLJ e-1-^'-: selective leach-) I .Ms- ••! ^^_ij,ljj Jl A ilj] ^JLC jl -., - ^I,.> ^ "t. 11L (ing
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Jl jlj-a] (Ji IJJ'IJ-LUI J j I -> - 1 (BDH 4^^ Cliil) j^l/rl^ NT. f ' (Prolabo (BDH (Dissolution of the yellow cake) tlja.^JI <£*SJ\ <_jlj]-\ , \./\ J^Uo^l^ 5JL ^J j I -* * ' <• w < ^ ( . .,y u < I ^ M *• .T.Jt (Precipitation of UO4) •> j- < • • ••<'< j^i - ." • '• 11 oUI JjU Jl X . V J.5* 0 f* 6_U_J I J 6-J •* I J -S ^J^ 1 j "'I > I f A . 0 «_£ I jj ^/ 0 \ ^ K. j " . » [ il ^v I I J l I I . I " V Y * , II VI - • / \ •<*"!• V2 1[ *j^jl jj_JI (Reduction of UO4 and obtaining of pure UO3) o'^ >' 11 I ^S _• - -j, " " I I * j > *' I j j * 1 I ^ • - .Xl ^jj-fl ^jl \ ^-l-i^-a- ^ aj '_*j -^ I I A n 1 i I . ft ) ) I _) 1 . . 1 ^ I A A fl A I • -N. ^J\ I > 1 1 til A 1 • 0 n t d 0 i I . .i I | (Chemical analysis) ^M ••_. A_J 4 1 '-^ 11 j^LiiJ o"i -> 11 £ Ijj jVI j jULj jL^a. *l J > "i. nL >_iLljaiJ I Jl ^ '^Ul ^L_^l J^ ^_JI ^ JJjj"(ICP-MS) *j-aJI ( .(Tris-2- ethyl hexyl phosphate) [o] il j— •» , .] Q i a rt 1 I ( ^| ft ^ | f tj \. \ A \ 4 **\. i t A I | f 1 31 ' j I ( l 1 A. fl ) J 9 ^ **^ ' I *y-A f • -^ ' 0 . • ' I A i *• ' I . • ^> I \ r . A • t j A n i \ \ . A I 1 | . ** i I fl i^) » A I i , i ft I Li /v I ) * .^ I r J *. i N . ^ t f. | .a . ss I I 4 \ t S. I ] p ^ -•>. | A i s , i i | n , .. I I J_J v •-v a , A ft t i /\ oj 2 I q A ft < i .. I IS, ) | ( A r, ^ } j > i I A »\ I I t i v i \ -s. I I . . f~j I \ r I H| ) i ..y I jJUoJ I IjAJ I ^ lie j f j^i I jj-J I J_* J j J* > . J^ \ % 1 1 j • -~ *• * 11 J.-.-..II J-^-H-11 M-g/g Mpm M-g/g u 62.58% As 180 Zn 40 B 10 Sr 5 Fe 1580 Na 150 Mo 560 Co 2 Mg 40 Cd 2 Ni 3 Al 220 Ba 8 V 5 K 60 Pb 10 Th 50 Ca 360 Ag 20 RE 6 Cr 10 Cu 20 S 150 Mn 30 Ti 75 - - ..I i - I 2 <.< I I v_, > , .'. I • j . 11 v_,lj_i — \ *:d_JLiJ| JI £^JI J-0 J J-A-t J J -I oJ I ,Jil fl'l T , X i-Jl j ^ I I *1 *fc *1 ^ I I ^j£ JLJJ-J_>^JI JJI -> i j_i jj — ^ j—J-I I j J j I I i . •. . * -1 •,!> *•>. ^1 > . ^ jf I > i r -f. I ) I <*• o , • i** i Lc I • -i \ , i. V I* -f4- \: —1\» < / > I - I j a .^11 »j_j_j I j J Jl X • X fc y M. -.V H. Jjl -> r, j J _e^( jj—^J I j ** i Lc LMJ t 1 t>°jj ajl ^-> d J^LLUI iVl^U 1^1"" I A II >. 5jlJA, <^ jj CJIXLLU *\ »J_oJ • • • I a ~i I I £_,, jjJ/j> I jJi. ^ X . ilj-jjl ^ljl,> . 5 ~ j "• * -'' • '' jjJiJIa-^.L>i*«Jltt*&JI3LtljjtJ-a^LJI ^^Jl M-g/g u 62.5 As 28 Zn 5 B ^j ' ~ j j ' _' 0II ,i j in^f Jjj-i Jjl ~ - J)l * jj -• *• -11 c^LujljjJI ^jjLii +2H2O -> UO4.2H2O + 2HNO3 (2) J ' _' I (JuV (/\.) U:j_aVl Jj I — LJLAJ IjJj J-.L.JI J^LiiJI (NH4)4 UO2(CO3)3 + 6HNO3 -> UO2(NO3)2 +4NH4NO3 +3H2O +CO2 ....(3) j 0 '^Jj' *() ^ J wit^) Jjj-fi ^pl] EDTA Jjl -> r> LflLbj J-AJLJ 11J A ,/jl ia-a.^Li cu-^ j . EDTA Jjl ~» n *-a *j ' ^ J j w^ ' ' .. .Xi j j_i * I ^ Hg/g^UI . -.11 •»l.--....l.v:-J-.H HO2O2 + EDTA Na HO2O2 1.9 Mg 14 2.1 Th 9 3 K ]j 10 Ca 48 5 Fe 66 10 Mn 112 <0.1 As 8 9 Zn 51 <0.1 Mo 3 7 Ag 150 <0.l 6 < . v. <1 jj—i jj-« ,_,' *• 11 »j • '• I jj -ll ' '•••<'< iiJI_j jrl_ljj SjLc ^JLJ de-) ^j.. -•. ,. Jlj" -^ j • t_> a '-II ^j_ijljj_JI 'j •••<] iiJLj ^Ic Jj .n-> II jkJj <-a.j"i,S o II »l i X ". ...I . 4 ijLaJI ^jlj ~ II <-^jJ (j-S f J •'•!jj -II * ' • •• 2Na2S2Q3 + UO4 + 3H2O -> Na2S4O6 + UO3+ 2NaOH ...(4) sod. thiosulphate sod. tetrathionate (XRD) «i JI'IJ 1.1 II (i) ^Sj Jj^-aJ . 2H2O) .4-1 IZJ Th Zn As Mn Mo Fe Ca Mg K Na 3.2 1.5 9.5 1.0 7.8 10.5 5.3 10 10.6 12 M-g/g e"•'»" ii II . J jJI I (jSL Lai .^-.11 t.r • jj_JI "i 11 w. •>. J J I -> ft f I .^ -> "l I nLj ^ J-J-J I J J-jJ I <_J I jj — N '• " 0 , 5j I 1 J-I-C CJH?-^' '* ju (/v\) j -1 _• 11 - vo. jn ft-., I ^lyiL Jb H 1 1 | i < 1 I | \ 1 . .[S. I A A fl • l . .. . 1 \ 4-sL^j - ; °' ' I (/o) EDTA J IJ Ml I I ' '^ JJlJ I I I -^ J.,.IJ..<-J J j»3_l_ll jJ_J I .i n.l'vl CJJLJ £-u>^-> ,»J_l I .1 I in^ I "^ fc A—i i. * , t . C I "i P ' f*> I 1 ^ ^ * ^ I I *>-0 i. t Jjl ~ - *'*JJ *'* ' .... I2>_a oJJ jij * «l^>t (jLaVl J>J> j i t^ jj^ LfJ j_al^_j_i LA_^ I (j 'ir JCJLJI ^ *• • -II VI tJliUi^^-l^S f • ** . ~" ^ j_*Lflb_aJ I (J * * •"• • ' ' j\ i ci ft j!^_^ Jj^o JjJxo-l liLJi^j < . JI * - "^ Co I * ~ **' * ••** d * ' ** • ^** ^3^ " * ^ JJ IJ (^^^ ^ £^ *—^ >J • *'J * 2 1 [1] C.R. Menit, The Extractive Metallurgy of Uranium, USAEC, CSM Research Inst., Colorado, p. 285, 1971. [2] IAEA, Proc. Tech. Comm. Metting on Advances in Uranium Refining and Conversion, Vienna, 1986. [3] E.M. El-Shazly and N.M.T.El-Hazk, Proc. of Symp. on Recovery of Uranium from its Ores and other Sources, IAEA, Sao Paulo, 1970. [4] W. Davies and W. Gray, Talanta, Vol. 11, p. 1203, 1964. [5] A.M. Abdallah, M.S. El-Alfy, E.M. Hussein and H.M. Serag, Determination of uranium and associated impurities in El-Atshan yellow cake, under publication. [6] A.K. Hammad, A.M. Abdallah and H.M. Serag, Production of nuclear pure uranium trioxide from El-Atshan yellow cake using Tri-n-Butyl Phosphate, Proc. 3rd Conf. on Chem. and its Role in Develop., Fac. of Science, Mansoura Univ., April, 1994. [7] A.K. Hammad, A.M. Abdallah and H.M. Serag, Preparation of nuclear pure uranium trioxide from El-Atshan crude yellow cake using Tri-Octyl Phosphine Oxide. Proc. 2nd Arab Conf. on the Peaceful Uses of Atomic Energy, Cairo, Nov. 1994. [8] E.M. Hussein, M.Sc. Thesis, Faculty of Science, Ain Shams Univ., 1997. [9] M. Shabbir and K.E. Tame, Hydrogen Peroxide Precipitation of Uranium, Rept. NO. 7931, U.S. Bureau of Mines, Salt Lake City, Utah, 1974. t.ot Jji ••"II 2lj ... *L3_ijJa <_i jjJj 1 >l in i (Jlj-ljJ—I....IJ in^j—Ljljj) ijlva _)-^-cj < t-> J "i J oLji_«_c J>La. ,j_o jiJij CjLjLa_iSJI j CJilkJI d^> Q "i • »j