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journal of NUCLEAR SCIENCE and TECHNOLOGY, 21[12J, pp. 949-958 (December 1984).

949

Reductive Extraction of Lanthanide and Actinide


Elements from Molten LiF-BeF2 Salt
into Liquid Bismuth
Hirotake MORIYAMA, Kunimitsu YAJIMA, Nobuaki NUNOGANE,
Tetsuo OHMURA, Kimikazu MORIT ANI and Jun OISHI

Department of Nuclear Engineering, Kyoto University*

Received May 9, 1984

The equilibrium distributions of several lanthanide and actinide elements between molten
LiF-BeF 2 salt and liquid bismuth were determined over a wide range of salt composition at
some temperatures from 600 to 800°C. The distribution behavior of each element was ap-
parently affected by salt composition and temperature. The effect of salt composition on
the distribution behavior was well explained by considering the formation of complex in the
salt phase. Also, the excess free energies of the solutes in the bismuth phase, calculated
from the equilibrium distribution data, were considerably negative, which suggests the for-
mation of intermetallic compound in the bismuth phase. Taking into account the formation
of these compounds, the equilibrium distribution can be expressed as
Licm-nJMF m+ n Li + x Bi = MBix + m LiF .
KEYWORDS: molten salt breeder reactors, chemical processing, reductive ex-
traction, molten fluorides, liquid metal, bismuth, rare earths, actinides, complex
compounds, intermetallic compounds, thermodynamics, equilibrium

I. INTRODUCTION
The molten salt breeder reactor (MSBR) developed first at the Oak Ridge National
Laboratory (ORNL) would be qualified as one of the most suitable type for the 232 Th- 233 U
fuel cycle 0 ' ' 2'. Among its many characteristics, the use of the circulating liquid fuel which
makes MSBR very different from the present reactors is the most important because of the
easiness of continuous chemical processing of the fuel. Effective chemical separation of
fission products and intermediate products 233 Pa leads to an improvement of the breeding
ratio in the fuel cycle.
Presently proposed method for processing MSBR fuel involves the reductive extraction
of these products from molten fluoride fuel into liquid bismuth 0 ' ,., . In support of the de-
velopment of the process, this type of extraction has extensively been studied by ORNL
researchers<sl-<GJ. They determined successfully the equilibrium distributions of various
elements between molten fluoride salt and liquid bismuth and showed chemical feasibility
of the reductive extraction for processing MSBR fuel. For the establishment of this process,
however, much more knowledge is needed on the reductive extraction.
Recently, the effect of salt composition on the equilibrium distribution of such typical
elements as thorium and radium between molten LiF-BeF 2 and liquid bismuth has been
studied by the authors' 7' <sl over a wide range of salt composition. In these works, the
distribution has been explained by considering the formation of complex in the salt phase.
* Yoshida-honmachi, Sakyo-ku, Kyoto 606.

-63-
950 ]. Nucl. Sci. Technol.,

The present study is an extension of our previous work to the lanthanide elements, lanthanum
and cerium, and the actinide elements, protactinium and neptunium, for a systematic com-
parison. In addition to the effect of the salt composition, the excess free energies of the
solutes in the bismuth phase are also discussed here.

II. EXPERIMENTAL
The apparatus and the general procedure employed in this study have been described
elsewhere' 7 >cs>. In a typical experiment, 200 g of bismuth and 50 g of salt were loaded in
a stainless steel or in a graphite crucible. Radioactive tracers 140 La, 143 Ce, 233 Pa and 239 Np
were produced by neutron irradiation of La, Ce, Th and U metals, respectively, at the
Kyoto University Research Reactor and added to the system. The system was heated to
a given temperature under an inert gas atmosphere.
The extraction of the solutes from the salt into the bismuth was effected by the incre-
mental addition of lithium as a reductant to the system. Lithium-bismuth alloy was added
to the system until a part of the solutes was transferred from the salt into the bismuth.
After a few hours of equilibration with gas sparging, the samples were taken out from
each phase with a stainless steel sampling tube under a reduced pressure. The radio-
activities in the samples were analyzed by a direct r-spectroscopy. The lithium in the
samples was analyzed by a flame photometry after dissolving the samples into nitric acid
solutions.

m. RESULTS
1. Material Balance
Except for protactinium, the material balance of each element was found to be satis-
factorily good during a few ten hours of experiments. A typical example for protactinium
is shown in Fig. 1. The protactinium balance was problematical since the total radioac-
tivity for 233 Pa decreased with time and its decreasing ratio varied from experiment to
experiment. The protactinium balance became worse with the increase of lithium amount
in all the cases, and most part of the escaping protactinium was found on the crucible
wall. Without the addition of lithium, the content of protactinium present in the salt phase
was found constant for a few ten hours studied. This behavior of protactinium was ob-
served regardless of the materials of crucible used, stainless steel or graphite. Thus, the
disappearance of protactinium might not be attributed to the formation of protactinium
oxide precipitates in the salt phase but to the adsorption on the crucible wall. This sup-
position was further confirmed by the fact that the protactinium balance was improved
remarkably as seen in Fig. 2 when zirconium behaving similar as protactinium was added
to the system as a carrier. The effect of the adsorption on the material balance is signi-
ficant in the case of tiny amount of material itself. In fact, the quantity of protactinium
used in the present study was so small (rvl0- 12 mol·cm- 3 ) that the adsorption might have
lowered considerably the concentration of protactinium in the liquid phase resulting in
poorer material balance. This effect would be almost negligible in the conceptual MSBR
fuel containing about 10-" mol· em - 3 of protactinium.
2. Equilibrium Distribution
The distribution coefficients for an element M and for lithium were determined by the
following equations, respectively :

-64-
Vol. 21, No. 12 (Dec. 1984) 951

La balanc~

Po balance

Ce balanc~
c
0
102 ~
'' \
10""2
c
0
~
_g
10-2

.
'' u :;;
:; 0
..0
'A ~ E
'' "
0 ~
\ \ , ............. -;,·;·i-;;-metal E
~u
u .r· ',, Li in m~tal
c"
.!'! 0
"
0 1 0

'~ 101
--! 10-3 ~
c
=g
a:
101
Li in metal

i Pain salt
"uc
0
u
i
i
i
i
/
10° '---LL.L.-'---'---'---L....-L...............J 10"" 4
0 4 6 7
Tim~. hr Time, hr

Fig, 1 Reductive extraction of protacti- Fig. 2 Reductive extraction of protactinium


nium from molten LiF-BeF 2 into from molten LiF-BeF 2 into liquid
liquid bismuth at 6oo·c bismuth at 6oo·c in presence of
0.5 g zirconium as carrier

DM=AM<Bi)! AM<F)' (1)

DLi=XLi(Bi)/ XLiF<F>' (2)


where AM is the molar radioactivity of the element M, XLi and XLiF are the mole fractions
·Of lithium and LiF, respectively, and the subscripts (Bi) and (F) denote the liquid bismuth
phase and molten fluoride phase, respectively. The obtained distribution coefficients for
each element are plotted as a function of the distribution coefficient of lithium in Fig. 3(a)""'
(d). The uncertainties involved in log DM and log DLi are about ±0.05.
IV. DISCUSSION
1. Effect of Salt Composition
As shown in Fig. 3(a)"-'(d), there are apparent effects of salt composition on the dis-
tribution behavior. These effects will be explained by considering the formation of com-
plexes in the salt phase as reported previously< 7>.
Assuming that the formation of complex for an ion Mn+ is essentially complete according to
MF n +(m- n)LiF=Li<m-n>MF m (m"?;n), ( 3)

the equilibrium distribution of the element M can be expressed as


Li<m-n>MFm+nLi=M+mLiF, ( 4)
where n denotes the valence of the element M. Equation ( 4 ) deduces the following rela-
tion: ( 5)

where DM=XM(Bi)/XLi<m-n)MFm<F>' ( 6)

K~=K4 h;<m-n>MFm(rLi)n/rM, ( 7)

-65-
952 ]. Nucl. Sci. Technol.,

0
() "' j
66.7
65.0
600'C
2


Q

""]
60:0
() 65.0
() 50.8
0 e 40.0 •
()
60.0
50.8
600'C

~ 65.0 700 'C


101 70.0 e 40.0

0 66.7 ~ 65.0 700'C

""]
-1 () 101
II 65.0
" ...J
• 60.0 . 0 66.7

~
0 u
0 II 65.0
"'
0 000'<
2"'
-1
• 60.0
-2

-3 -2

-4 -3
-5 -4 -3 -2 -5 -4 -3 -2
log Du
log Dli

(a) Lanthanum (b) Cerium

2
Q


'M]
66.7
60.0
600'C

'"']
Q

0 66.7 () so.o
600'C

()
60.0
so.o
101
D
roo]
66.7
aoo•c
• 60·0

"']
101
ll so.o
D 66.7
BOO'C
0 • 60.0

I
ll so.o
0
"
a.
0
a.
z
2"' 2"'
-1
-1

-2

-5 -2
log Du log Du

(c) Protactinium (d) Neptunium


Fig. 3(a)-(d) Distribution coefficient of lanthanum, cerium, protactinium and
neptunium between molten LiF -BeF 2 and liquid bismuth

-66-
Vol. 21, No. 12 (Dec. 1984) 953

K 4 is the equilibrium constant of reaction ( 4) and a and r are the activity and the activity
·Coefficient of the species concerned, respectively. The DM defined by Eq. ( 6) is essentially
the same as that in Eq. ( 1 ). In the systems investigated, each component in the bismuth
phase was present at very low concentration (<0.01 m%) and so the values of TM and TLi
are considered to be practically constant. Since Licm-n>MF m is present at low concentra-
tion (<0.01 m%) in the salt phase and interacts no longer with the solvent, TLicm-n>MFm
may also be treated as a constant. This means that K~ is a constant value at a given
temperature. The term (n log XL;F-m log aL;F) in Eq. ( 5) depends only on the salt com-
position. Thus, a plot of log DM vs. log DLi gives the straight lines having a slope of n
for each salt composition. Figure 3(a)'"'-'(d) show that lanthanum, cerium and neptunium
are present as trivalent and protactinium is in tetravalent state in the salt phase.
Figure 4 shows the plots of log [DM/(DLi)n] vs. XLiF for several elements in this
work and in others' 4 ' ' 7 ' . The most suitable
values of m and log K~ in Eq. ( 5) have soo•c
been determined for each element with the
sets of log [DM/(Ddn] and XL;F and the
known values for TL;F' 9 ' by the least squares 15
method, and are shown in Table 1. The
{:Urves in Fig. 4 are drawn with the deter- .,
<;...
mined values of m and K~. It was shown 0
:J

that all the trivalent elements, lanthanum, "-0:::<: TO


cerium and neptunium, have m values L-1
Cl
around 3 and the effect of salt composition .£

on their extraction behavior is similar to


each other. The distribution behavior of
5
tetravalent protactinium was affected by the
salt composition similarly as the tetravalent
thorium (7). Thus it can be concluded that
the effect of salt composition on extraction
OL-_ _L__ _L__ _L___!__ _!__...J.____.J
behavior is not so different among the 0-3 0.4 0.5 0.6 0.7 0.8 0.9 1-0
elements having the same valence, while XLiF
the effect is very different among those The data of thorium and radium
having the different valences. The for- are taken from Ref. (7).

mation of complexes in the salt phase Fig. 4 Effect of salt composition on equili-
brium distributions of various ele-
seems to depend largely on the valence n. ments from molten LiF-BeF2 into
This should be a measure of polarizing liquid bismuth at 6oo·c
power.
2. Excess Free Energy of Solutes in Liquid Bismuth
The formation of complexes in the salt phase has a significant influence on the extrac-
tion behavior as described above. On the other hand, the formation of intermetallic com-
pounds in the bismuth phase can be expected to take part in the equilibrium distribution.
In order to estimate this effect, the excess free energies of various solutes in the bismuth
phase are calculated from the equilibrium distribution data with the aid of the available
thermodynamic data.
The standard Gibbs free energy change .tJc• for the reaction shown by Eq. ( 4) is
given by
-67-
954 ]. Nucl. Sci. Techno/.,

Table 1 Parameters obtained from equilibrium distributions of lanthanide


and actinide elements between LiF -BeF 2 and bismuth

Salt composition Temp. Para met erst


(m% LiF) ("C) Element - --···--· ·----- -----
n log [DM/(DLi)n] m logK~

40.0 600 La 3 8.91 2.90±0.11 6.11±0.10


50.8 8.41
60.0 7.81
65.0 7.34
66.7 7.33
70.0 6.82
65.0 700 La 3 6.52 2.82 5.37
66.7 6.36( 4 )
60.0 800 La 3 6.30 3.54±0.19 4.24±0.12
65.0 5.73
66.7 5.62
70.0 5.18
40.0 600 Ce 3 9.42 2.96±0.12 6.52±0.11
50.8 8.94
60.0 8.18
65.0 7.80
66.7 7.67
70.0 7.38
-----------· ------------------ ----- --------
65.0 700 Ce 3 6.99
60.0 800 Ce 3 6.81 3.66±0.33 4.61±0.19
65.0 6.10
66.7 5.98
70.0 5.61
50.0 600 Np 3 12.05 3.27±0.28 9.11 ±0.22
60.0 10.99
66.7 10.52
70.0 10.00
50.0 800 Np 3 10.04 3.30±0.24 7.36±0.18
60.0 9.11
66.7 8.51
70.0 8.25
50.0 600 Pa 4 16.11 5.78±0.80 10.38±0.63
60.0 13.77
66.7 13.09
70.0 12.26
----~-

50.0 800 Pa 4 12.92 5.91±0.37 7.77±0.27


60.0 11.21
66.7 10.19
70.0 9.50
t The uncertainties listed are the standard deviations.

-68-
Vol. 21, No. 12 (Dec. 1984) 955

LJc• =mLIG((LiF)-LIG((Licm-n>MF m)
=-RT InK,, (8)
where LIG{(LiF) and LIG{(Licm-n>MF m) are the free energies of formation of LiF and
Licm-n>MF m• respectively. The excess free energy LIG~ of solute M in the bismuth phase,
which is relative to each metal state, is expressed as follows by combining Eqs. ( 7) and ( 8) :
LIG~=RT In rM
=-mLIG;(LiF)+LIG;(Licm-n>MF m)-RT InK~
+RT In hicm-n>MFm +nRT In rLi. (9)
An approximation is introduced to estimate LIG~ according to Eq. ( 9 ). Since Licm-n>MF m
present at low concentration in the salt phase interacts no longer with the solvent,
rLicm-n>MFm is considered to be unity. Table 1 shows that all the trivalent elements (n=3)
have m values around 3 and that they exist mainly as MF 3 in the salt phase. Consequently,
Eq. ( 9) is simplified for the trivalent elements as
LIG~~-3LIG((LiF)+LIG;(MF 3 )-RT In K~+3RT In rLi. (10)

The excess free energies of the trivalent elements in the bismuth phase were calculated
by Eq. (10) with the aid of the data for the equilibrium distribution, the free energies of
formation° 0' - ' 15 ', and h;, which was given by Ferris et al. for dilute solution of lithium in
bismuth'''. The results are summarized in Table 2. The excess free energies of the
divalent elements shown in Table 2 have also been calculated by a similar equation assum-
ing that m=2. As shown in Table 1, on the other hand, the tetravalent elements have m
around 6 and exist mainly as Li 2 MF 6 in the salt phase. The excess free energies of the
Table 2 Excess free energy of solutes in liquid bismuth

Temp. LIGJ (MFn) Ll G~ (kcal;mol)


M n logK~
c·c) (kcal/mol) Present Literature
La 3 600 6.11 -361. 22(11) -56.17 -47.14° 6 '
700 5.37 -355 .47°1) -56.50
800 4.24 -349. 73(11) -54.18
Ce 3 600 6.52 -361. 27 02 ' -57.87 -43. 94° 7 '
700 5.73 - 355. 59° 2' -58.20
800 4.61 -349. 92° 2 ' -56.19
Nd 3 600 6.65! - 356. 36° 2 ' -53.48
Sm 2 600 3.97! -255 .4703 ' -51.69
Eu 2 600 3.09! - 265 .4803 ' -58.19
Gd 3 600 5.06! - 355 .47° 2 ' -46.23
Dy 3 600 4.51! -355 .44°'' -44.01
Th 4 600 7 .1( 7 ) -32. 92c18)
Pa 4 600 10.38 -26.00° 9 '
800 7.77 -25. 97° 9 )
u 3 600 11.05! - 296. 99° 5 ) -11.68 -15.58C 20)
Np 3 600 9.11 -309.55!! -16.49
800 7.36 -298.68tt -18.45
Pu 3 600 10.Ut -322.11 (15) -33.05 -32.36( 2!)

Estimated from the distribution data"' using Eq. ( 5) with an empirical value of 2 or 3 for m.
For lack of experimental data, use of analogy with compounds of neighboring elements in the
periodic table was employed.

-69-
956 ]. Nucl. Sci. Technol.,

tetravalent elements could not be calculated in the same manner because of the lack of
information on the free energy of formation .JG;(Li2MF6). In spite of the approximation
used, some calculated excess free energies are found to be in fair agreement with those in
literatures 06 J-< 21 J and this indicates the validity of the present treatments.
Although the values of the excess free energy of the lanthanide and actinide elements
vary with element, they are apparently negative in all cases. These negative values sug-
gest the presence of strong interactions between the elements and liquid bismuth. It has
been known that the lanthanide and actinide elements from various intermetallic compounds
with the elements having incomplete p shell such as bismuth <22 ) <2sJ. The negative excess
free energies might thus be attributed to the formation of some intermetallic compounds
in the bismuth phase as
M+xBi=MBix. (11)

Assuming that the formation of intermetallic compound is complete like as that of complex
in the salt phase, the equilibrium distribution of Eq. ( 4) can be rewritten as
(12)
It is of interest to follow the change of the excess free energy with element for having
an insight to the nature of the intermetallic
La Ce Pr Nd Pm Sm Eu Gd Tb Dy
compound. Figure 5 shows the excess
free energies of the trivalent elements to-
gether with the free energies of formation
of their fluorides. The change of .JG~ with
60 t-........_,L
~~ , ... ....
______ __ - 360
"() ' ,
.
50 t- ' 350
element is apparently similar to that of '
'-o- ___ 0 -
.JG£(MF 8 ). This correlation might suggest 0 40 t- - 340 0
that the bonding characteristics of the ele- E
...... ~
- 330 "
Ci ~
ment M in the intermetallic compounds are u
30 t-
""'
considerably similar to those in the tri- UJ:;[
(!)
;r
fluorides. This leads to the fact that the <I 20 t- - 320 :;[
I (5'"
separation factors among the elements hav- <I
10 1- - 310 I
ing the same valence, especially among the
elements neighboring in the periodic table, 0 r- - 300
are not so high. Although further theoretical
studies are required for complete under- -10
Ac Th Pa U Np Pu AmCmBk Cf
290
standing of these intermetallic compounds, The temperature is 600"C.
the correlation in Fig. 5 could provide a Fig. 5 Excess free energy of trivalent ele-
useful means for estimating the .JG~ values ments in liquid bismuth and free
of which data are lacking. energy of formation of trifluorides
3. Rate of Reductive Extraction
From the practical technological point of view, the rate of reductive extraction is very
important since it affects directly the efficiency of extraction. Some preliminary experi-
ments were carried out to clarify the kinetics of reductive extraction. These experiments
were performed under the condition that the contact areas between both phases were
narrow and so the equilibrium distributions were attained more than ten hours later after
the addition of reductant. As a typical example, Fig. 6 shows the rate of reductive
extraction of lanthanum. An important phenomenon observed is that the rate of increase
of lanthanum concentration in the bismuth phase is somewhat lower than that of decrease
-70-
Vol. 21, No. 12 (Dec. 1984) 957

in the salt phase. This leads to the break


of material balance of lanthanum. The
90
similar phenomena have been observed for
the other elements and can be explained :§ 80
\\ ,....#-· ---------
2 1 I La in m~tal
by assuming multi-step reactions. In view ~
I I
0 \ I
• 70 I
of Eq. (12) for the equilibrium distribution, I
"" -\
I /
the reductive extraction might be controlled ; 60
--/
by the possible two reactions such as 1:
c
\ I
.c I _i
Li<m-n)MF m+nLi---+ M+mLiF, (13)
~ 50 \I I /
0
I
XI
M+ xBi---+ MBix . (14) .::-40 , I
·;; ' I I
The metal M which liberates according to ~ 30 \ i \
0 ~' .I 'I
reaction (13) might be supposed to be ad- 'C
c 'I, ' Li in m~tal
sorbed on the crucible wall and then be dis- a: 20 i --------~----
i ',,
solved gradually into the bismuth phase by 10 ! ',.... __
La _in salt

reaction (14). The lower rate of increase i ------


of lanthanum concentration in the bismuth o L---'-----'--'-___~_--'----'---'---'--'-----'O.oo
0 4 8 10
phase could be interpreted by supposing Time, hr
that the rate of reaction (14) is slower than Abscissa represents the time elapsed after
that of reaction (13). the addition of reductant lithium.
For clearer elucidation of the mechanism Fig. 6 Reductive extraction of lanthanum
of the reductive extraction, further investiga- from molten LiF -BeF2 into liquid
bismuth at 600oC
tions will be necessary.
V. CONCLUSIONS
The following conclusions can be drawn in the present study on reductive extraction
of lanthanide and acitinide elements from molten LiF-BeF 2 into liquid bismuth.
(1) The equilibrium distribution of each element depends on salt composition and tem-
perature.
(2) The effect of salt composition is well explained by considering the formation of
complexes in the salt phase.
{3) The excess free energies of solutes in the bismuth phase are considerably negative,
indicating the formation of intermetallic compounds between the solutes and bismuth.
(4) Equilibrium distribution may be expresssed as

Li<m-nlMF m+nLi+xBi=MBix+mLiF.

ACKNOWLEDGMENT
A part of this work was done under the Visiting Researchers' Program of the Kyoto
University Research Reactor Institute. The authors wish to thank Prof. T. Tarnai and
Messrs. S. Nishikawa and A. Koyama for their interest and encouragement. They also
acknowledge the financial support of a Grant-in-Aid for Energy Research of the Ministry of
Education, Science and Culture.
-REFERENCES--

(1) WEINBERG, A.M., et al.: Nucl. Appl. Technol., 8, 105 (1970).


(2) RosENTHAL, M. W., HAUBENREICH, P. H., BRIGGS, R. B.: ORNL-4812, (1972).
(3) FERRIS, L. M., MAlLEN, ]. C., LAWLENCE, ]. ]., SMITH, F.]., NoGUERA, E. D.: ]. Inorg. Nucl.

-71-
958 ]. Nucl. Sci, Technol.,

Chern., 32, 2019 (1970).


(4) FERRIS, L. M., MAlLEN, J. c., SMITH, F.].: ibid., 33, 1325 (1971).
(5) FERRIS, L. M., SMITH, F. J., MAlLEN, J. C., BELL, M. J.: ibid., 34, 313 (1972).
(6) FERRIS, L. M., BREDIG, M.A., SMITH, F. J.: ]. Phys. Chern., 71, 2351 (1973).
(7) MoRIYAMA, H., YAJIMA, K., ToMrNAGA, Y., MoRITAMI, K., OISHI, J.: Nucl. Techno!., 62. 133
(1983).
(8) idem: Proc. 1st. Int. Symp. on Molten Salt Chemistry and Technology, Kyoto, p. 419 (1983).
(9) HITCH, B. F., BAES, Jr., C. F.: Inorg. Chern., 8, 201 (1969).
(icy STEINMETZ, E., RoTH, H.: ]. Less-Common Metals, 16, 295 (1968).
~l) REZUKHINA, T. N., SJSOEVE, T. F., KHOLOKHONOVA, L.l., IPPOLITOV, E. G.: ]. Chern. Thermo-
dynamics, 6, 883 (1974).
M KHOLOKHONOVA, L.l., REZUKHINA, T.: Z. Fiz. Khim., 50, 767 (1976).
M HAMER, W. J., MALMBERG, M.S., RUBIN, B.: ]. Electrochem. Soc., 112, 750 (1965).
(14) REZUKHINA, T. N., SrsOEVA, T. F.: ]. Chern. Thermodynamics, 11, 1095 (1979).
(151 BROWN, D.: "Halides of the Lanthanides and Actinides", p. 244 (1968), John Wiley and Sons,
London.
(16) KOBER, V.I., LEBEDEV, V. A., NICHKOV, I. F., RASPOPIN, S. P.: Z. Fiz. Khim., 42, 688 (1968).
(17) idem: ibid., 45, 569 (1971).
(18) WrsWALL, Jr., R. H., EGAN, J, J.: Proc. Symp. on Thermodynamics of Nuclear Materials, p. 345
(1962), IAEA, Vienna.
(191 FERRIS, L. M. : !nor g. Nucl. Chern. Lett., 1, 791 (1971).
(20) LEBEDEV, V. A., NrcHKov, I. F., RAsPOPIN, S. P.: Z. Fiz. Khim., 42, 690 (1968).
(21) LEBEDEV, v. A., BABIKOV, L. G., VAVILOV, S. K., NICHKOV, I. F., RASPOPIN, s. P., SKtBA, 0. v.:
At. Energ. (USSR), 27, 59 (1969).
(22) BAYANOV, A. P.: Uspekhi Khim., 44, 236 (1975).
(23) MARDON, P. G. : "Comprehensive Inorganic Chemistry", Vol. 5, p. 103 (1973), Pergamon Press,
Oxford.

Errata (Vol. 21, No. 11 (1984))

Page As printed To read

815 Eq. ( 2) F(r, r,)=)JCr, r)dr F(r, r,)= )JCr, r)s(r, r,)dr

-72-

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