ORNL-TM-3763.txt

 

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J”\EQ: ‘ for the
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ORNL- TM- 3763
ESTIMATED BEHAVIOR OF TITANIUM IN MSBR
¥ CHEMICAL PROCESSING SYSTEMS
o L. M. Ferris
NOTIC is document contains information of a preliminary nature
v and qusT:repufed prim::rily ;or interia! u;e at :he Ozk |Ridge );lm‘ionul

Loboratory. It is subject to revision or correction and therefore does
not represent a final report.

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This report was prepared as an account of work sponsored by the United
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subcontractors, or their employees, makes any warranty, express or implied, or
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ORNL-TM-3763

Contract No. W-7405-eng-26

CHEMICAL TECHNOLOGY DIVISION

Chemical Development Section B

ESTIMATED BEHAVIOR OF TITANIUM IN MSER
(JHEMICAL PROCESSING SYSTEMS

L. M. Ferris

NCTICE

This report was prepared as an account of work
sponsored by the United States Government. Neither
the United States nor the United States Atomic Energy
Comimission, nor any of their employees, nor any of
their contractors, subcontractors, or their employees,
makes any warranty, express or implied, or assumes any
APRTL 1972 legal liability or responsibility for the accuracy, com-

pleteness or usefulness of any information, apparatus,
product or process disclosed, or represents that its use
would not infringe privately owned rights.

 

 

 

OAK RIDGE NATTIONAL LABRORATORY
Oak Ridge, Tennessee 37830
operated by
UNION CARBIDE CORPORATION
for the
U.S., ATOMIC ENERGY COMMISSION
1ii

CONTENTS
Abstract + ¢« 4 e« ¢ ¢ o 4 2 o s o & e A & 2 3 o e + e s g + v e
1. Introduction ¢ ; e ¢ ¢« = ¢ 5 o 3 ¢ ¢« a © s o o ¢ & o » ¢ o
2. Thermodynamliec Treatment . o ¢ ¢« « o & ¢ ¢ 5 2+ o & o o 5
3, Leaching of Titanium from Titanium-Modified Hastelloy into
Fuel Salt + & s ¢ o o = ¢ 8 o @ = s ¢ s a s = a o & 3 o o
4. FEstimated Behavior of Titanium During Fluorination of MSER

O Co 1 O\

O

Fuel Salt o s ¢ ¢ e o 0 © o ¢ o o ¢ 5 = s 8 & 8 a4 5 o e s
Behavior of Titanium in Reductive Extraction Processing .
Estimated Behavior of Titanium During Hydrofluorination .
Behavior of Titanium in Oxide Precipitation Frocesses . .
Acknowledgments . ; ¢ ¢ s o o o ¢ o o « o s e s < o s o &

References G < - < o v . - @ # [ w € < . * . r & - . ® 2 o

O Oy

13
13
1L
 
ESTIMATED BEHAVIOR OF TITANTUM TN MSBR
CHEMICAL PROCESSING SYSTEMS

I, M. Ferris
ABSTRACT

Available thermodynamic information was used to estimate
the behavior of titanium in a fluorination--reductive extrac-
tion flowsheet for processing MSBR fuel salt. It was first
shown that titanium is likely to be leached from a titanium-
modified Hastelloy N containment vessel into a LiF-BeFp-
ThF,-UF) fuel salt at 600°C, The primary reactlon would
probably be 3 UFl(4) + Tl(Hastelloy{ = TiF + 3 Uk l
The estimates showed that, during I'luorina 1on, T1F wou d
be oxidized to TiF). A large fraction of the TiF) would be
expected to volatilize during fluorination. Any titanium
not volatilized by fluorination would be present in the salt
that enters the reductive extraction step. Experimental
data confirmed the prediction that titanium would be prac-
tically quantitatively extracted from the salt in this step.
It was also shown that titanium can be transferred from a
bismuth phase to a salt phase by oxidation with gaseous HF,
and that HF is not a sufficiently strong oxidant to convert
TiF3 to TiFuf

KEY WORDS: *MSBR, *Processing, *Modified Hastelloy N,
*Titanium, fused salts, fluorination, reductive
extraction process.

 

1, INTRODUCTION

Hastelloy N (68% Ni--17% Mo--7% Cr--5% Fe) was used® for the con-
tainmment vessel and other metallic components in the Molten-Salt Reactor
Experiment (MSRE). However, use of a modified Hastelloy containing up
to 2 wt % titanium is being considered® for molten-salt breeder reactors
(MSBRs) since an alloy of this type is expected to be more resistant to
radiation embrittlement than Hastelloy N, In the event that a suitable
alloy is developed, it is of interest to know what extent titanium will

be leached from the alloy into the molten salt and, if the extent of
leaching is significant, how titanium will behave in an MSBR chemical
processing system. The present reference flowsheet®'® for chemically
processing an MSER involves, first, fluorinating the salt to remove
uranium as UFg and, then, contacting the resultant salt with ligquid
bismuth containing about 0.002 mole fraction each of lithium and thorium
to remove protactinium by reductive extraction. The rare earths remain
in the salt during these process steps and are removed in a subsequent
metal transfer process. Protactinium and other elements extracted into
bismuth will subsequently be transferred to a sglt phase by hydro-
fluorination of the bismuth in the presence of the salt. The purpose
of this report is to estimate the behavior of titanium both in the
reactor system and in the various chemical processing steps. The es-
timates, which were made using the general thermodynamic treatment
developed by Baes,* could be compared, in some cases, directly with

experimental results,
2. THERMODYNAMIC TREATMENT

Baes®* has summarized a large amount of equilibrium data involving
molten LiF—BeF2 solutions in terms of standard half-cell potentials
(E°) referred to the reaction HF(g) + e = F-(d) +1/2 Hg(g)’ for which
E° is defined as zero at all temperatures; (g) and (d) denote gaseous
and dissolved species, respectively., The standard state for most solutes
is the hypothetical unit mole fraction ideal solution in LiF-BeF2 (66,7~

333 mole %); The exceptions are LiF, BeF Be2+, Li+, and F_; the

’
activity of each of these species is defingd as unity in the reference
salt composition. With LiF-BeF, (66.7-33.3 mole %) as the standard
state, the activity coefficients for solutes are unity, whereas
Ypap = 12 804 Ypp, = 3

The potential for a complete reaction is obtained by algebrailcally
adding the necessary half-cell reaction potentials. For example, at
600°C the equilibrium of pure crystalline chromium metal with UlL+ dis-
solved in LiF-BeF, (66.7-33.3 mole %) can be expressed as the algebraic

sum of the twec half-cell resactions:
 

Cr =Cr" + 2 e : E° = 0.4 v (1)

(c)
U 4 2 e” = pudT 3 B = 21,1467 (2)
Cr( gy * 0 = Bt 4 g3t . E° = -0.746 V (3)

The standard free energy change for reaction (3) is:
AG® = -zFE° = (-2.3RT) log K |, (%)

in which z is the number of faradays, I' is the Faraday constant, R is
the gas constant, T is the absolute temperature, and K is the equilibrium
constant. For our purposes, we will assume that E° values (and K's derived
from them) are the same in LiF-BeF,-ThF), (72-16-12 mole %), the composition
of the MSBER carrier salt, as they are in LiF-BeF, (66.7-33.3 mole %). A1l
estimates included in this report were made at 600°C.

The electrochemical behavior of titanium species in molten fluoride
salts has been studied voltammetrically by Manning.® From this work,

Manning® estimates the following at 600°C:

Tiot 4 3/2 Wiy = Tiggy + 3/ w2t ®° - 21.8+0.1V  (5)

't L1/ iy = 133t 1/ mAt . E° =0.2 £0.05V  (6)
Combining Fg. (5) with

3/2 Wit + 3 e = 3/2 Ny 3 E = 0,368V (7)

yvields

7137 4 3 &7 = iy 3 B0 =-LA3E0.17. (8)
Similarly, from Egs. (6) and (7) we obtain:

13t o™ et E° = -0.568 £0.05 V . (9)

Use of Egs. (8) and (9), along with values of E° for other appropriate
half-cell reactions, allows estimation of the behavior of titanium in a

molten-~salt reactor system and in the associated chemical processing plant.

3. LEACHING OF TITANTUM FROM TITANIUM-MODIFIED
HASTELLOY INTO MSBR FUEL SALT

The question of whether titanium will be leached from g modified
Hastelloy into an MSBR fuel salt at a significant rate is a difficult one
to answer since the overall rate of leaching would depend both on the
rate at which titanium diffuses to the surface of the alloy and on the
oxidizing power of the salt. Of the species present in the salt, ULL+ is
the most likely oxidant for titanium. The reaction would probably be:

Ti oy + 3 o33ty w3, P -o0.286%017 ,  (10)

for which log K = 4.94 + 1.7, since the reaction producing Tiu+, given

below, is thermodynamically much less favorable:

Lt bt

i) * yutt - bt 4w : ° = ~0.282 * 0.15 V . (11)

The value of log K for reaction (11) is -6.5 * 3. Comparison of the E°
for reaction (10) with that of reaction (3) confirms earlier predictions®
that titanium would be much more reactive than chromium to oxidants in

the fuel salt. Despite the fact that the thermodynamic driving force

for the leaching of titanium from a modified Hastelloy N is much greater
than that for the leaching of chromium, it is nearly impossible to es-
timate the thermodynamic activity of titanium at the surface of the alloy.
Not only will the concentration of titanium in the bulk alloy be less than
one-third of that of chromium (about 2% vs 7%) but also the diffusion

coefficient for titanium in Hastelloy N is about a factor of 10 lower
than that for chromium.’ Thus, the titanium activity at the Hastelloy
surface at a given time should be considerably lower than the chromium
activity. Only direct experimentation can show whether the activity is
low enough to offset the large driving force represented by the E° for
reaction (10).

An experimental study conducted several years ago by DeVan and
Evans® provided evidence that titanium might be leached from Hastelloy N
at a higher rate than chromium. In their studies, cast alloys of Ni--17%
Mo containing up to 8 wt % of an additive were made into tubing from
which thermal convection loops were fabricated. These loops were exposed
to NaF-LiF-KF-UF) (11.2-45.3-41.0-2.5 mole %) for 500 and 1000 hr. The
hot-zone temperature of each loop was 815°C, and the cold-zone temperature
was 650°C. After each test, the salt was chemically analyzed for the
additive. The corrosion susceptibilities (i.e., the amount leached) of
the additives increased in the following order: iron < nioblium <
vanadium < chromium < tungsten < titgnium < gluminum, With the excep-
tion of tungsten and niobium, the susceptibilities increased in the same
order as did the thermodynamic stabilities of the fluoride compounds of
the respective elements. Tt is significant to note that the rate of
leaching was much higher during the 500-hr period than during the 1000-hr
period. This result suggests that nearly steady-~state conditions were

established within the first 500 hr.

4., ESTIMATED BEHAVIOR OF TITANIUM DURING
FLUORINATION OF MSBR FUEL SALT

In this and the ensuing sections, it will be assumed that titanium
is present in measurable concentrations in MSBR fuel salt that enters
the chemical processing plant. As noted in Sect. 1, the first chemical
processing step is fluorination of the salt to remove uranium as UF6.

Lt

Fluorination should result in the gquantitative oxidation of Tisf to Ti :

Ti3t 4 1/2 Folg) = TR : E° = 2.30 £ 0.1V , (12)
for which log K = 13 £ 1. Reaction (12) can also be written as:
TiF + 1/2 F_ = TiF . 1
F3(a) * /2 Ta(g) = Ty(q) (23)

Since the boiling point of TiF) is only about 28L4°(C,? it is probable that
a significant fraction of the titanium would be removed from the salt as
TiFu during fluorination and would accompany evolved UF6 to the fuel
reconstitution step. An example of the inherent tendency of TiFh to
volatilize from fluoride melts is provided by the experience of Manning
et 21.2° They found that, after K,TiFy was added to molten LiF-NaF-KF
or LiF-BeFZ-ZrFu solutions at 550°C, TiFh volatilized from the melt and.

condensed on cooler parts of the system.
5. BEHAVIOR OF TITANIUM IN REDUCTIVE EXTRACTION PROCESSING

Any titanium not removed during fluorination will be present in the
salt that enters the reductive extraction step®’® for protactinium isolation.
In this step, the salt is contacted with a liquid bismuth stream containing
about 0,002 mole fraction each of lithium and thorium, Protactinium,
residual uranium from the fluorination step, zirconium, and some of the
noble-metal fission products are transferred to the bismuth phase in this
step.

The extraction into liquid bismuth of a solute MF,, present in low
concentration in molten LiF-containing salts, can be expressed as the
general reaction:

MFn( ) +n Li(

& pr) = Mmy) * R Iy (14)

in which (d) and (Bi) denote the salt and bismuth phases, respectively.

This reaction is the sum of the half-reactions
Mn+ +ne =M (15)

nli=nli +ne . (16)
The standard potential for reaction (14), i.e. the algebraic sum of the
potentials for reactions (15) and (16), is related to the equilibrium
constant as follows:

n
_ %L . (aFE° /RT)

n 3y
ME 214
n

K (17)

a

in which a is activity and the other symbols are as defined previously.
By letting a = Ny (where N is mole fraction and y is an activity co-
efficient) and by defining the distribution coefficient for a given

element as Dy = Ny/Nyp , it was shown by Ferris'! that
n

1
log K = log Dy - n log D . = (nFE®/2.3RT) + n log (7Li/7LiF)

i
- log (ry/71:m) - (18)

With LiF-BeF, (66.7-33.3 mole %) as the salt phase, Baes®* defined Yiip =
n

log K, = (nFE®/2.3RT) + n log Yrs - O log(1l.5) - log Ty (19)
or, at 600°C,
! o
log Ky = n(5.773)E° - 0.176n + n log yrq - o8 7y (20)

In order to calculate log Kfi for a given element, we obviously need
values of the activity coefficients Y14 and 7y that are referred to the
pure metals as the standard state, in addition to the appropriate E°
values. Values of E° for a large number of solutes are available from
Baes;? those for titanium species were estimated by Manning.® Values of
y11 and yy for several solutes were taken from the literature and were
summarized by Ferris et gi.lg These values of yrj and yy are for very

dilute solutions of M in liguid bismuth. No information on the activity
coefficient of titanium in liquid bismuth could be found in the literature.
Thus we will assume that Y4 is equal to yp,.. Workers at Brookhaven National
Laboratory obtained!?® Yy = 0.012 at 700°C. If we assume that the excess
chemical potential “gr = (2.3RT) log vz does not change throughout the
temperature range 600-700°C, we can calculate log yy, = log yps = -2.1 1
at 600°C.

From the above sources, we obtain E° = 1.224 £ 0.1 V at 600°C for the

reaction
TiFB(d) + 3Ly =3 LiF(d) +Ti (21)

and, using Eq. (20), estimate log Kéi3+ = 10.4 * 2 with LiF-BelF, (66.7-
33.3 mole %) as the salt phase., Table 1 compares this value and the values
for other selected solutes with values obtained experimentally using LiF-
BeF,~ThF), (72-16-12 mole %) as the salt phase. The values of log Kér and
log Kfi are those measured earlier by Ferris et al.,'* whereas the value

of log Kéi was determined in the course of the present work. Note that

the values of log Kfi obtained for LiF-BeF,-ThF) (72-16-12 mole %) are
somewhat higher than those calculated for LiF-BeF, (66.7-33.3 mole %).

Table 1. Comparison of Values of log Kfi Calculated for LiF-BeF
(66.7-33.3 mole %) with Those Determined Experimentally at 600°C
for LiF-BeFp-ThF) (72-16-12 mole %)

 

 

 

log Kfi
Calculated for Megsured with

log 7y E° LiF-BeFy LiF-BeFp-ThF),
M 1 (V) (66.7-33.3 mole %) (72-16-12 mole %)
Ii 1 -h.13 - - _
7r L -2.1 1.226 13.2 =1 14,7 £ 0,3
U 3 -3.87 1.143 10,7 = 1 11.1 * 0.2
Ti 3 -2.1 1.224 10.4 % 13.6 £ 0.b

 
The experiment to determine the value of log Kéi was conducted using

the general procedure outlined previously.'® This experiment was initiated
by simultaneously hydrofluorinating, in g molybdenum crucible, LiF-BeFE-
ThF),~CsF (71.7-15.9-12-0.4 mole %) and bismuth containing dissolved titanium.
This treatment resulted not only in the transfer of the titanium to the
salt phase but also in the removal of oxide from the system. With the
system at 600°C, thorium was added in increments to effect the reductive
extraction of titanium from the salt into the bismuth phase. At least 2k
hr was allowed for equilibration after each thorium addition before filtered
samples of the respective phases were removed for analysis. The salt and
metal samples were anglyzed for titanium by a colorimetric method:; the
lithium concentration in the metal phase was determined by flame photometry.
Data from this experiment are summarized in Table 2, and a plot of log
Dry
determination of the value of n. However, thermodynamic considerations

vs log Drs is shown in Fig. 1. The scatter in data points precludes

(Sect. 6) strongly indicate that n should be 3 (and not 4). The value of
log K%i3+ = 13.6 £ 0.4 is the mean of the values calculated from each data
point. This value is somewhat higher than the estimated wvalue (Table 1);
however, the agreement is good, considering the uncertainties in the
thermodynamic quantities used. Furthermore, the experimentally determined
value of log K%13+ is consistent with the results of an earlier experiment
by Moulton gfi_géo,ls which indicated that log Kéi3+ should be greater than
log K&3+. In their experiment, it was found that titanium dissolved in
bismuth did not effect detectable reduction of either U3* or Fa* from
LiF-BeF,-ThF), (72-16-12 mole %) at 600 to T00°C.

During the chemical processing of MSBR fuel salt, it appears certain
that titanium, if present in the salt entering the reductive extraction
step, will be quantitatively extracted into the bismuth stream along with

protactinium and other easily reduced species.
6. ESTIMATED BEHAVIOR OF TITANIUM DURING HYDROFLUORINATION

Tn the reference MSBR chemical processing method,®*2 the bismuth
phase from the reductive extraction step used to isolate protactinium

would be treated with an HF-H2 mixture in the presence of a salt phase
10

Table 2. Distribution Coefficients and Values of log Kf13+
Obtained at 600°C from Measurements of the Equilibrium
Distribution of Titanium Between Molten LiF-Belp-Thf)-CsF
(71.7-15.9-12-0.4 mole %) and Liguid Bismuth Solutions

 

 

Sample lO6 NLi lO5 DLi DTi log Kéi3+
3 8.73 1.218 0.038 13.3
6 16.0 2.226 0.435 13.6
7 18.7 2.60k 0.695 13.6
8 16.6 2.310 1.06 13.9
9 27.4 3.822 1.31 13.4
10 20.8 2.898 1.76 13.8
11 20.5 2,856 2.33 14.0
12 33.7 L. 704 3.88 13.6
13 65.0 9.072 5.9k 12.9

1L 28.3 3.948 15.7 1h. 4

 
11

ORNL DWG 72-32I0

 

 

 

 

! l l b T
O
10— =
e O-..
- = -
z
5V] = —
=2 O
o -
u O
& O O
z Lo ]
o C :
— " -
2 = -
9 -
s
- _ ~
0
O
S F
=
=
fio.l_—_—' —
N .
— O ~
| | l [ 1 ] ]
oo, 2 3 4 5 6 7 8910
10°D;

Fig. 1., Equilibrium Distribution of Titanium Between Molten
LiF-BeF_-ThF, -CsF (71.,7-15.9-12-0.4 mole %) and Liguid Bismuth
Solutions at 600°C.
12

to oxidize protactinium and other elements present in order to effect -
their dissolution in the salt phase. Since titanium could be one of the
elements initially present in the bismuth phase, its behavior during
hydrofluorination is of interest.

The reaction of primary interest is:

3 HF(g) + Ti(c) = 3/2 Hz(g) + TiF E° = 1.k3 0.2 v , (22)

3(a)  ?

for which log K = 25 = 2 at 600°C., Despite the fact that the activity
coefficient for titanium in liquid bismuth is of the order of 10'2, thermo-
dynamic considerations led us to expect titanium to be easily hydrofluorinated
from a bismuth phase into a molten fluoride salt phase. This expectation
was confirmed (at least under one set of conditions) in the initial phase
of the experiment described in Sect. 5. In this experiment, bismuth and
LiF-BeFgp-ThF) -CsF (71.7-15.9-12-0.4 mole %), contained in a molybdenum
crucible, were simultaneously hydrofluorinated at 600°C to remove oxides
from the gystem. After sparging with purified argon, sufficient titanium
metal was added to give a titanium concentration of 2500 wt ppm in the
bismuth phase. Analysis of a sample of this phase confirmed that all the
titanium was dissolved in the bismuth. The two-phase system was then
sparged at 600°C for about 20 hr with HF-H, (50-50 mole %). Analyses of
the respective phases showed that all of the titanium had been transferred
to the salt phase during the hydrofluorination period.

Gaseous HF does not appear to be a sufficiently strong oxidant to
convert T13+ to Tiu+; consequently, hydrofluorination of a bismuth-salt

system should leave the titanium in the salt as TiF This conclusion

30
is based on the following estimate at 600°C:

IS

3+ _ . - o _ _ +
Ti”" + HF(g) =1/2 Hg(g) + T+ F E° = -0.59 £ 0.05V , (23)

e

for which log K = -3.,3 * 0.3, Since the activity coefficients for the
solutes are defined as unity, the expression for the equilibrium constant

for reaction (23) will give:
13

(W /W 34) = K(pHF/piéz) . (2h)

Expressing the partial pressures in atmospheres, we find that, even with

 

nearly pure HF as the gas phase, the equilibrium concentration of Tiu+ is
extremely low as compared with the Ti3+ concentration:
pHF/pHZ Bopg /My 3+
1 0.0004
10 0.002
100 0005

7. BEHAVIOR OF TITANTUM IN OXIDE PRECIPITATION PROCESSES

Oxide precipitation is being studied as an alternative to fluorination--
reductive extraction for isolating protactinium and subsequently removing
uranium from MSBR fuel salt.?® Protactinium would be precipitated as
Pa205;17'18 consequently, the salt would have to be treated with an oxidant
such as HF to convert Pau+ to Pa5+ prior to the precipitation step. As
shown in Sect. 6, HF is not a sufficiently strong oxidant to convert TiSt
to Tiu+. No information could be found in the literature on the behavior
of Ti3* in molten fluoride salts containing dissolved oxide. Experimental
work would be required to determine this behavior,.

Some information on the apparent sclubility of Ti05 in fluoride melts
is available. Mailen®® had indications that TiO, was less soluble than
U0z in LiF-BeF,-ThF), (72-16-12 mole %) at 600°C. Similarly, Bamberger and
Baes®® equilibrated TiO, with LiF-BeF,-ThF) (72-16-12 mole %) at 600°C.

The equilibrium titanium concentration in the salt was about 40 wt ppm,

which 1s lower than the solubility of U0, in this salt.
8. ACKNOWLEDGMENTS

The author thanks J. F. Land for conducting the experimental portion
of this work. Analyses were provided by the group of W. R. Taing, ORNL

Analytical Chemistry Division,
10.

11.

12.

13.

14,

15,

14

9. REFERENCES ~—

H. E. McCoy et al., Nucl. Appl. Technol. 8(2), 156 (1970).

L. E. McNeese, MSR Program Semiann. Progr. Rept. Feb. 28, 1971,
ORNL-4676, p. 234.

W. L. Carter, E. L. Nicholson, and L. E. McNeese, MSR Program
Semiann. Progr. Rept. Aug. 31, 1971, ORNL-4728, p. 179.

C. F. Baes, Jr., "The Chemistry and Thermodynamics of Molten Salt
Reactor Fuels,' in Nuclear Metallurgy, Vol. 15, ed. by P. Chiotti,
CONF-690801 (1969), p. 617.

 

 

 

D. L. Manning, ORNL, personal communication, Nov. 19, 1971.

W. R. Grimes, Nucl. Appl. Technol. 8(2), 137 (1970).

H. E. McCoy, ORNL, personal communication, Feb. 22, 1972,

J. H. DeVan and R. B. Evans III, "Corrosion Behavior of Reactor

Materials in Fluoride Salt Mixtures," in Corrosion of Reactor

 

Materigls, Vol., II, p. 557, IAEA, Vienna, 1962.

C. D. Hodgman (ed.), Handbook of Chemistry and Physics, 36th ed.,
p. 614, Chemical Rubber Publishing Co., Cleveland, 195k,

 

D. L. Manning, F. R. Clayton, and G. Mamantov, in Anal. Chem. Div.
Research and Development Summary - Dec. 1971, ORNL-CF-72-1-11

 

 

(Jan. 6, 1972), p. 1k.

L. M, Ferris, Some Aspects of the Thermodynamics of the Extraction

 

of Uranium, Thorium, and Rare Earths from Molten LiF—'BeF2 into
Liguid Li-Bi Solutions, ORNL-TM-2486 (March 1969).

 

L. M, Ferris, J. C. Mailen, and F., J. Smith, "Estimated Free Energies
of Formation of Some lanthanide and Actinide Halides at 600°-800°C
Using Molten Salt-Liquid Metal Distribution Coefficient Data,” J.
Tnorg. Nucl. Chem. 34, 491 (1972).

R. H. Wiswall, Jr., and J. J. Egan, Thermodynamics of Solutions of
Actinides and Fission Products in Bismuth, BNL-6033 (1962).

 

 

L. M. Ferris, J. C. Mailen, J., J. Lawrance, F. J. Smith, and H. D.
Nogueira, J. Inorg. Nucl. Chem. 32, 2019 (1970).

D. M, Moulton, J. H. Shaffer, and W. R, Grimes, MSR Program Semiann.
Progr. Rept. Feb. 28, 1970, ORNL-L4548, p. 176.

 
16.

17.

18.

19.
20.

15

M. J. Bell and L. E. McNeese, MSR Program Semiann. Progr. Rept.
Feb. 28, 1971, ORNL-4676, p. 237.

R. G. Ross, C. E, Bamberger, and C. F. Baes, Jr., MSR Frogram
Semiann., Progr. Rept. Aug., 31, 1970, ORNL-L622, p. 92.

0. K., Tallent and F. J. Smith, M3R Program Semiann. Progr. Rept.
Aug. 31, 1971, ORNL-4728, p. 196,

J. C. Mailen, ORNL, unpublished results.

C. E. Bamberger and C. F. Baes, Jr., MSR Program Semiann. Progr.

Rept. Feb. 28, 1970, ORNL-45u48, p, 1hO.
o

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Bamberger
Beall

Bell
Bennett
Bettis
Blanco
Blankenship
Boyd
Briggs
Brooksbank
Brown
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Culler
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51-52.
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56-58,
59.

McCoy
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Nichols
Nicholson
Perry
Rosenthal
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Dunlap Scott
shaffer
Skinner
smith
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Taylor
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Trauger
Weeren
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Youngblood
Central Research Library
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Laboratory Records
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