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ORNL-4224.txt
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3 4y5L 0515828 1
i
|
ORNL-4224
Contract No. W-7405-eng-26
CHEMICAL TECHNOLOGY DIVISION
Chemical Development Section B
FLUORINATION OF FALLING DROPLETS OF MOLTEN FLUORIDE
SALT AS A MEANS OF RECOVERING URANIUM AND PLUTONIUM
J. C. Mailen and G. |. Cathers
NOVEMBER 1968
QAK RIDGE NATIONAL LABORATORY
Oak Ridge, Tennessee
operated by
UNION CARBIDE CORPORATION
for the
U. S. ATOMIC ENERGY COMMISSION
N
|
i
3 445k 0515828 1
|
CONTENTS
A ract v v ittt e e e e e e e e et et e e e e e e e,
1. IbrodUch On o v i e st e e e e e e e e e e e e e e e e e
2. Experimental ... ... e
2.1 Fluoride Salts Used .. .. ... oo,
2.2 Apparatus and Procedure ... ... Lo o oL,
2.3 Velocity and Time of Fall of Droplets . .. .. ........ ...
3o Resulis o v ot ot e e e e
3.1 Sorption of UiFé and F‘tuF6 on the Surfaces of Frozen Droplets .
3.2 Fluorination of Uranium=Containing Salfs .. ...........
3.3 Fluorination of Plutonium-Containing Salts . .. .. .. .. ...
3.4 Fluorination of Protactinium=Containing Salts . . .. .. ... ..
4. Possible Applications . ... ..o i i i e e e
4.1 Removal of Uranium from Molten=Salt Breeder Reactor Fuel . .
4.2 Processing of Low-Enrichment Reactor Fuels . .. ... ... ...
5. Acknowledgments . . . .. ... e
B, References. . v v i v v i i e e et e e et e e e et e e e e e
o W NN
FLUORINATION OF FALLING DROPLETS OF MOLTEN FLUORIDE
SALT AS A MEANS OF RECOVERING URANIUM AND PLUTONIUM
J. C. Mailen and G. |. Cathers
ABSTRACT
A falling=drop fluorination method was devised for the recovery of
vranium and plutonium from molten fluoride salts. This method, in which
molten-fluoride droplets fali countercurrently through fluorine, has sev-
eral advantages over methods in which fluorine is bubbled through the
melten salt. Among these are: (1) higher removai rotes for both uranium
and plufonium, {2) lower rates of corrosion of the containment vessel
{(since the molten salt does not contact the wall), (3} the possibility of
continuous operafion, and {4) minimal corrosion-product contamination
of the fluorinated salt. The low corrosion-product content and longer
fluorinator life are especially attractive from the standpoint of molten~
salt reactor processing, where the fluorinated saly must be recycled to
the reactor and the fluorinator must be very duroble.
Experimental equipment was developed, and small-scale fluoring~
tion experiments were made, using several salt solutions. With the
data obtuined from these experiments, we caiculated that, by using a
5-ft-long fluerination column at 650°C, 99.9% of the uranium can be
removed from 100~ ~diam droplets of Molten-Salt Breeder Reactor fuel.
With an 11-ft-long tower at 840°C, 99% of the plutonium caon be re-
moved from 100-1~diam droplets of salt.
» - - - a e 23!
In similar experiments using salt droplets containing = Pa, no
protactinium was fluorinated, even ab temperatures as high as 614°C.
1. INTRODUCTION
In the molten~salt fluoride volatility process} and in molten-salt reactor fuel
processing,2 uranium and/or plutonium are removed from molten fluoride salis by
fluorination. Sparging of a pool of molten salt with fluorine would appear to be the
simplest method, but it results in undesirably high c:or:_'c;ssis.‘:nr'a:3 of the vessel ond o low
2 4 . . .
rate of plutonium removal.” The later is caused, in part, by the thermodynamic
necessity, at 600°C, to have at least 69 moles of fluorine in the gas for each mole of
PUF6 in order to overcome the tendency of the plutonium to remain as nonvolatile
PUF4- However, o falling-drop fluorinator circumvents both problems. In it, corrosion
is reduced because only small amounts of molten salt contact the fluorinator well, and
rates of fluorination are high since diffusion distances are short. This is particularly
advartageous for plutonium since the fluorinesplutenium atem ratio is inherentiy high
in the fluorinator.
A spray-fluorination system for recovering uranium from molten fluoride salt
was previously studied by other workers.é In this method, the molten fluoridae mixture
was sproyed downward into a fluorination tower. The moximum uranivm removal ob-
tained was obout 30%. This low removal is partiolly attributed to the contact of the
molten droolels with "cold" Flucrine {maximum temperature, 200°C), which permitied
Il
tham to solidify too soan. Also, the gas flow was concurrent with the salt flow, thus
allowing b‘-é in the gas to sorb on the frozen salt purticles. In our studies, the
fluoride salt mixture wos pulverized and then dreppad into o fluorination tower, where
the particles melted and were contacted with fluorine, flowing upward through the
tower, of 500 to 700°C. This approach resulted in much higher recoveries.
2. EXPERIMENTAL
2.1 Fiuoride Salrs Used
In experiments in which the fluorinction of plutonium was studied, the solvent
salt was Nab-Zrf , (50-50 mele %) containing either .026 or 2.58 mg of plutonium
~J
(as PUF*B per g of salf.
Six different compositions were used in experimenis involving uranivm:
1. NafF-ZrF ~UF (48.75-48.75-2.5 mole %)
4 7 4
2. NaFerF4"lJF (48-48-4 mole %)
3. NOF"Z!’F4 UF (45.5-45.5-9 mole %)
4. NoF~ZrF - (37.4-56.1-6.5 mala %)
4
5. NaF~LiF—ZrF4-UF4 (31.7-31.7-31.7-5 mole %)
b. E_iF-BeF2 (66-34 mole %) containing 9.4 mg of uranium per g of salt
The salt used in the protactinium experiments consisted of NuF—ZrF4 {50-50
mole %) containing about 0.25 mg of 233% per g of salt.
2.2 Apparaius and Procedure
The main parts of the equipment for the falling~drop fluorination experiments
involving plutonium and protactinium {Fig. 1) were: a powder feeder, a preheater
section; o 52-in.~leng fluorination section, and a salt receiver. In addition, there
were the necessary gas supplies and regulators, electrical heaters and controls, traps
for fluorine and PuF ./ and glove boxes for piutonium ond protactinium contoinment.
The equipment used for experiments involving uranium was essentially the same, except
that glove boxes were not required. A.iso, in the experiments with uranium, fluorination
sections of different lengths (28, 44, and 56 in.) were used.
The procedure consisted in pulverizing and sizing the fluoride salt, and then
feeding the sized powder through the glass feeder (Fig. 2), by turning a nickel~wire
helix, into the preheater section of the column. (Helium flowing through the powder
feeder protected it from fluorine and served os a blanket gas for the preheater section
of the column.) The small drops (58 to 210 K in diameter) of molten salt, obtoined
when the sized powders were melted in the preheater section, then fell through the
fluorination section. In some of the experiments with uranium, lorge drops {cbout
3000 L in diometer) were produced directly by means of o high~temperature pipet.
Before the start of each experiment, the column was flushed, first with helium,
admitted at both the top ond botiom of the column, and then with helium and fluorine
(equal velumetric flow rotes) admitted at the top ond the bottom of the column, respec~
tively. During each experiment, the fluorine and helium flow rotes were also kept
equal.
After passing through the fluorination section, the "depleted™ salt drops were
frozen ond collected in a stainless steel cup located in the bottom of the column. In
GAS EXIT__|
DIP- LINE
SIX CLAMSHELL
HEATERS
ORNL DWG.68-87¢
TO SECONDARY TRAF
AND 0; F-GAS HEADER
s e FDT— 7
TRAP FORF,
/AND PuF, *
T
—
1
|
|
|
|
=L2F?PER GLOVE BOX
|
o
. — v e ToREETT. man
s
COOLING WATER
e
IPREHEEHNG SECTION
LFLUORINAT iON SECTION
-
b
@ COOLING WATER
oomemrerresoodiiin
j~——t-COLLECTION CUP
}Lowm GLOVE 80X
Fig. 1. Equipment for Fluorinating Failing Droplets of Plutonium-Containing
Salts. Apparatus for recovering uvranium waos essentially the same.
ORNL.-OWG 68~7627
| |
POWDER RESERVOIR
HELIUM k ) - TEFLON 5SLUIP JOINT
\ ‘“1 r NICKEL ROD
\(MQQ,QJLSQM_QQMQQQ
\ NICKEL WIRE HELIX
SWAGELOK FITTING
—
& A WITH TEFLON FERRULES
SCREW FEEDER FOR POWDERED
FLUCRIDE SALT (TURNED BY HAND)
V0 | Ll L LA
TOP FLANGE
Fig. 2. Powder Feeder.
almost all of the experiments with uranium~containing salt, this cup contained «
chilled liquid fluorocarbon to prevent UFé in the gas from sorbing on the frozen
salt. After collection, the frozen droplets were sieved; then, the different size
fractions were sampled for chemical analysis.
2.3 Velocity and Time of Fall of Droplets
The velocity of the droplets must be known in order to calculate the time of
contact in the fluorination tower. The velocity of 137-L-diom droplets falling
through fluorine ot 00°C was calculated as a function of time, using drag coefficients.
Figure 3 is a plot of these colculated velocities. At 600°C and 1 ofm, the falling
droplet reaches its termina! velocity of sbout 60 cm/sec after falling only 8.7 em.
Thus, the important velocity for the droplets (except for the 3000~ droplets, which
do not attain terminal velocity in o short fall) is the terminal velocity. Terminal
velocities for particles of other sizes were eosily calculated because, for small drop~
lets, the terminal velocity is nearly proportional to the square of the diameter. Since
most of the fluorination experiments were done ot &00 + 50°C, the rate of fall was not
corrected for temperature. In these experiments, the residence time of a small drop
in the fluorination tower can be expressed as:
t (sec) = ......__,,.l:mwm.,._u ;
¢ 1,246 x 107 d”
where d is the porticle diameter in microns, ond L is the length of the fluorination
section in inches.
3. RESULTS
3.1 Sorption of UFé and PuF, on the Surfaces of Frozen Droplets
6
Since, in our system, the frozen salt was collected in the bottom of the folling-
drop tower, it wos necessary to examine the possibility that uranium and plutonium
hexafluorides were being sorbed on this salt and biasing the experimental results. In
ORNL DWG.68-882
M W o (8! D
o o o o O
!
VELOCITY {CM/SEC)
o
o b b b oo 1oy
TERMINAL VELOCITY
TIME (SEC) DISTANCE TRAVELED (CM)
0.02 0.1786
0.086 ).33
.10 3,10
0.14 5.19
0.18 7.51
0.20 8.6
TIME (SEC)
Fig. 3. Calculated Rate of Fall of 137-u~diam Salt Droplets in Fluorine
af 800°C and 1 aim.
O
0 002 004 006 008 0IO 012 OM Qs 0i8
most of the uranium experiments, the droplets were caught in a poel of chilled liquid
fluorocarbon, which prevented direct contact between the frozen salt and the UFéa A
significant increase in uranium removal was obtained in these runs, particularly when
the particle diameter wos large (Fig. 4); the maximum removal without use of the
fluorocarbon was about 99.5%, whereas the maximum removal with its use was greater
than 29.9%.
In the plutonium work, this procedure was not used because the potential hazaid
of contacting fluorine with a fluorocarbon was considered to be too great. If it had
been used, some sorption on the frozen salt undoubtedly would have been orevented.
However, by analogy with the uranium results (Fig. 4), only 1 to 2% of the
volatilized plutonium would have been expecied to sorb on the frozen droplets. Since
less than 88% of the plutonium was volatilized in any experiment (Sect. 3.3), surface
sorption would change the amount of plutonium found in o drop by less than 15%. This
is less than the experimental variation.
The data shown in Fig. 4 suggest that, in o large-scale falling-drop fluorination
tower, some method of preventing contact of the gas and the depleted salt would be
desirable. Probably the best solution would be to admit fluorine at the bottom of the
column at a flow rate sufficient to prevent significant amounts of UFé and PuF, from
b
contacting the solidified salt.
3.2 Fluorination of Uranium-Containing Salts
Table 1 shows a few examples of the data obtained in these experiments. In
general, the recoveries increased with decreasing particle diameter and with increasing
temperature, other conditions being the same. The uvranium recovery data obtained
with the six salt compositions were correlated by using the following equation:
_ 2, ~o/T
T/CU ]/CO,U (kt/D")e , (n
where
D = droplet diameter, 1,
T = fluorination temperature, °K,
3 3 8 DRNL DWG. 64-7511
;;5“
Q
<
0
= ®
2
ol
s
-
Z
<
5 |~ @ COLLECTED UNDER LIGUID FLUOROCARBON, C_F
816 o 0
g2l— O COLLECTED IN DRY CUP
_ NUMBERS BESIDE POINTS ARE NUMBER OF DATA POINTS COINCIDING
gob Lt v ooy b v bbb i
40 60 80 100 120 140 180 18O 200 220 240
DROPLET DIAMETER { !
Fig. 4. Removal of Uranium os a Function of Droplet Diameter Using
Different Methods for Collecting the Frozen Droplets.
10
Table 1. Results of Uranium Falling-Drop Fluorinations
in o 4-in.~long Fluorinator
Inttial salth NaFerF‘4 (50-50 mole %) containing UF
4
[nitial Firnal
Uranium Range Uraniuim Uranium
Corc. in of Drop Conc. in Remaoved
Salt i emp Diametars Salt from Salt
(ppm) (°C) (1) (ppim) (%)
170,000 554 88105 1,700 99.
105-125 2,7GC 98.4
125149 2,700 94.3
149177 21,9CC 87.1
54,400 559 63-38 202 99.6
88-105 212 99.6
105~125 419 99.2
125~149 1,724 96.8
80,000 530 ~3200 74,600 5.6
80,000 582 ~3200 74,200 7.2
51,800 638 125149 75 99.9
149177 126 99.8
177-210 260 99.5
186,000 640 105-125 70 99.96
125-149% 65 99.96
149177 99.91
162
I~
T T —
11
t = fluorination time, sec,
Co U= initial uranium concentration in the salt, wt fraction,
¥
CU = final uranium concentration in the salt, wt fraction, and
k and @ are empirical constants.
Values for log k and @ are given in Table 2, and plots of Eq. (1), using data for four
of the salt compositions, are shown as Fig. 5. In Fig. 6, the empirical constants are
plotted vs the liquidus fempemfufeB of the salt. No explandation for the lineor
relationships between log k and the liquidus temperature and between @ and the
liquidus temperature is known,
All the results indicate that, in a 4-ft~long fluorination column at 650°C, more
than 99.5% of the uranium con be removed from droplets that are less than 200 U in
diameter.
3.3 Fluvorination of Plutonium=-Containing Salts
Toble 3 summorizes the results of seven experiments in which NcF-ZrF4
(50-50 moie %), containing either 0.026 or 2.58 mg of plutonium {added as PUFB}
per g of salt, was fluorinated. The salt may not have been completely molien of
506°C because this temperature is below the liguidus temperature of the salt (510°C).
The dota from these experiments are correlated in Fig. 7, which consists of plots of
the fraction of the plutonium removed vs drop diometer. These constant-iemperature
plots are linear, and at the higher temperafures, the diamerer dependence is low.
Thus, plutonium removal is most efficient of high remperatures where the size of the
droplets is not a critical parameter. The following empirical equation correlates the
plutonium removal date, and con probably be used to predict removals within the
temperature range of these experiments:
F= (-5.04+7.65 x 107° T)d - 0.22T + 236 ,
where
F = plutonium removed, % (fluorinator length, 52 in.),
T = fluorination temperature, °C, and
d = droplet diameter, 1 .
12
Table 2. Correlation Constants for Equation (1) for Six Salts
Containing Uranium Tetrafluoride
Weight
Salt Composition Fraction Liquidus
(mole %) Uranium Temp. of Salt
NaF LiF ZrF4 UF4 BeF2 In Salt (°C) Log k o
X ]04
31.7 317 317 5 0.132 475° 15.78 1.45
48.75 48.75 2.5 0.0542 510 21.58 2.84
48.0 480 4 0.0843 515 21.58 2.84
45.5 455 9 0.1733 550 28.79 4.35
37.4 56.1 6.5 0.119 630 40.25 7.16
66.58 0.13 33.29 0.00942 480 15.00 1.42
a .
By cooling curve.
13
ORNL DWG. 64-7513 A
409‘
O
ke"a/-r
i
107
108
| I | I
¢ M NaF-LiF-ZsF 4~ UF
I
{ I
(31.7-31.7-31.7-5 mole %)
Liquidus temp., 460°C -
NaF-ZrF4~UF
(48.75-48.75-2.5 mole %)
Liquidus temp., 510°C
® NaofF-ZrF ~UF
(48-48-4 mole %)
Liquidus temp., 515°C
A NaF-ZrF -UFy,
(45.5-45.‘}5-—9 mole %)
Liquidus temp., 550°C
o ]
110 144
1.18 122
1/T x 10° (°K")
Fig. 5. Plots of Equation (1), Using Data Obtained with Four Salts.
14
ORNL DWG S8-887
451~
40 - — 8
35 -7
30 - o ~1 6
25 -5
6 =
20 t- / /—~-—m~ — 4
15 - / B -3
[
i -1
0 ! ! 1 1 ]
400 450 500 550 600 650
SALT LIQUIDUS TEMPERATURE (°C)
Fig. 6. Plots of Liguidus Tempercture of the Salt vs Constants from
Equation (1) for Salt Solutions Containing Uranium.
s XIO™4
15
Table 3. Results of Fluorination of Plutonium in Falling Molten-Salt Droplets
Initial salt: NaF-ZrF4 (50~50 mole %) containing PuF3
Length of fluorinator: 52 in.
Initial Final Plutonium
Average Range of Plutonium Plutonium Removed Fluorination
Temperature Drop Diameters Concentration Concentration From Salt Time
(°C) (W) (mg/a) (mg/a) (%) (sec)
528 88-105 0.026 0.020 22.9 4.5
105-125 0.0223 14.3 3.2
125-149 0.0220 15.3 2.2
570 88-105 0.026 0.0098 62.1 4.5
105125 0.0171 34.4 3.2
125-149 0.0209 19.7 2.2
149-177 0.0205 21.0 1.6
624 63-88 0.026 0.0156 40.0 7.3
88-105 0.0055 79.0 4.5
105-125 0.0088 66.0 3.2
506 63~88 2.58 1.232 52.2 7.3
88~105 1.45 43.8 4.5
105~125 1.58 38.7 3.2
125~149 1.09 57.8 2.2
149177 1.34 48.2 1.6
543 53-63 2.58 0.79 69.5 12.4
63-88 1.19 53.8 7.3
88-105 1.56 39.3 4.5
105125 2.04 21.0 3.2
609 53-63 2.58 0.45 82.7 12.4
63-88 0.50 80.4 7.3
105~125 0.93 64.0 3.2
125~149 1.06 58.8 2.2
640 53-63 2.58 0.33 87.4 12.4
63-88 0.32 87.6 7.3
88-105 0.39 85.0 4.5
105-125 0.48 81.3 3.2
PLUTONIUM REMOVED {%)
16
ORNIL. DWG 68-888
LENGTH OF FLUORINATION
100 |- COLUMN, 52 INCHES
20
80
T PLUTONIUM CONCENTRATION®
OPEN POINTS= 2.58mgAk
o0+ SOLID POINTS = 0.026mglg
0 1 1 { | ] 1 - } 1. i 1 J
50 60 70 80 90 100 10 120 (30 (40 B0 160 (70
DROP DIAMETER {u)
Fig. 7. Plutonium Removal as o Function of Drop Diameter at Constant
Temperature. Length of fluorinator, 52 in.
17
The plutonium removal in a tower having a length other than 52 in. can be estimated
from the following equation:
F1/100 = 1 - (1 - £/100)"752
where
F = plutonium removed in 52~in.-long fluorinator {drop diameter and
temperature constant), %,
F' = plutonium removed in fluorinator of length L', %, and
L' = fluorinator length, in.
3.4 Fluorination of Protactinium=-Containing Salts
Two fluorination experffmeni's, at 547 and 614°C, were made using NmF-‘ZrF4
{50-50 mole %) containing 231 Fa. Gamma counting was used for analysis of the
protactinium. No detectable amount of protactinium was volatilized in either
axperiment. However, the fluorine used throughout this entire investigation contained
obout 10 vol % impurities, including about 1% oxygen. The studies of Sirein9 at
Argonne National Laboratory indicated that, when the oxygen concentration in
fluoring is this high, nonvolatile PUEOFS is formed in preference to the more-
volatite PaF _.
5
4. POSSIBLE APPLICATIONS
4.1 Removal of Uranium from Molten-Salt Breeder Reactor Fuel
One possible application of the falling~drop fluorination scheme is for processing
Molten-Salt Breeder Reactor {MSBR) fuel. This fuel contains about 1.6 wt % uranium
and must be processed at the rate of about 16 frs/doyi {p=20 g/’cms). The total fuel
salt volume will be about 680 F?3 and will contain about 6.2 x 105 g of uranium. The
annual increase in uranium due to breeding will be about 7%. For procedures yielding
a 99% removal of uranium in the reprocessing step (assuming that the other 1% is lost),
we calculate that the annual foss of uranium would be about 2.6% of the total charge,
which is more than one~third of the uranium that is produced by the reactor. Thus,
18
processing schemes that do not permit recovery of at least 99.9% of the uranium would
be considered as economicolly infeasible. Using a falling~drop fluorinater having «
fluorination section that is 5 fi long (to keep the unit relatively compact), we cal-
culated that the moximum diameters of drops from which 99.9% of the uranium could
be removed at temperatures of 600, 650, and 700°C would be 90, 112, and 137 14,
respactively.
Drops of these sizes can be generated using a two-fluid spray nozzle. With
such a nozzle, the Unit Operations Section of the Chemicol Technology Divisimm
has succeaded in producing dronlets, most of which are 25 to 100 U in diomster.
Significantly, several thousand volumes of driving gos per volume of molien salt are
required to obtuin droplets of this size. Nitrogen has been proposed as the diiving
gos since fluorine is too corrosive to the spray nozzle; however, such o quantity of
inert gas in the fluorination tower would dilute the effluent fluorine too nuch fo
allow its recycle. In Molten-Salt Breeder Recctor fuel processing, disposal of the
unraccted fluorine probably would not be prokibitive since, for 309% utilization, this
would amount to only about 7500 Ib/yecr. Another approach might consist in forming
droplets {using a two-fluid spray nozzle}, freezing them in an inert afmosphere, and
feeding the frozen droplets into the top of o fluorination tower. This mathed would
require ¢ suitable mears for removing decay heaot from the frozen droplets to prevent
premature melting.
4.2 Processing of Low~[nrichment Reactor Fuels
At the present fime, it appears unlikely that molten-salt volatility mei‘hods]
will be used for processing reactor fuels that contain plutorium. If such processing
is contemplated, it should be noted that the falling-drop method is the only approach
thot has shown promise for the rapid removal of plutonium with low reaction-vesse!
corrosion rates. For example, our experimental dota indicote that fluorination in an
11-f-high tower will result in the removal of 99% of the plutonium from 100-H-diam
drops at 640°C. This corresponds to a fluorination time of about 11 sec. In the proc-
essing of salt containing plutonium, the fluorine would probeb!y have to be recycled
19
in order to maintain a high fluorine:PuF, mole ratic in the exit gas from the column
b
(to prevent decomposition of the PuFé). Recycling the fluorine would, in turn, require
that the droplets be formed in o separate tower, where the driving gas for the spray
nozzle would not dilute the fluorine in the fluorination tower. The drops would then
be frozen and fed to the top of the fluorination tower.
5. ACKNOWLEDGMENTS
The authors wish to acknowledge the assistance of 1. R, Knox, T. E. Crabtres,
aond H. F. Soard in the initial work on uranium falling-drop fluorination; and, the
valuable contributions of the enfire Process Design Saction, especially 3. B. Ruch,
io the design of the plutonium faliing~drop equipment. Gratitude is also expressed
1o the Analyiicol Chemistry Division for performing the many chemical anolyses for
uranium and plutonium,
&. REFERENCES
1. G. I Cathers, Nucl. 5¢i. Eng. 2, 768-77 (1257,
W. L. Carter and M. E. Whatley, Fuel and Blaonket Processing Development for
Molten Salt Breeder Recctors, ORNL-TM-1852 {June 1967).
{\3
3. A.P. Litman ond A. E. Goldman, Corrosion Associoted with Fluorination in the
Qak Ridge National Luboratery Fluoride Volotility Process, ORNL-2832
(June 5, 1561).
4. G. 1. Cathers and R L. Jolley, Recovery of PuF, by Fluorination of Fused Fluoride
Salts, ORNIL~3298 (Sept. 24, 19671,
5. A.E. Florin et al., J. Inorg. Nucl. Chem. 2, 368 (1956).
6. J. D. Gabor et al., Spray Fluorination of Fused Salt as o Uranium Recovery
Process, ANL~6131 (Morch 1961).
20
7. ). H. Perry (ed.), Chemicul Engineering Handbook, pp. 1018-20, McGraw-Hill,
New York, 1950.
8. S. . Cohen, W. D. Powers, and N. D. Greene, A Physical Property Summary for
ANP Fluoride Mixiures, ORNL-2150 (Aug. 23, 1956).