ORNL-TM-2335.txt

A RECEWVED 2 07k 107 1opg -

 

   

o operated by
- UNION CARBIDE CORPORATION
NUCLEAR DIVISION
for the
U.S. ATOMIC ENERGY COMMISSION
ORNL- TM- 2335
. SOLUBILITY OF CERIUM TRIFLUORIDE IN MOLTEN MIXTURES OF
LiF, BeF,, AND ThF,
o

at

NOTICE This document contains information of a preliminary nature
and was prepared primarily for internal use at the Ock Ridge National
Laboratory. It is subject to revision or correction and therefore does
not represent a final report.

WSTRIBUTION OF THIS QQCUMEND & UNUMITED
 

 

 

LEGAL NOTICE

This rsport was prepared as an account of Government sponsored work. Neither the United States,

nor the Commission, nor any person octing on behalf of the Cemmission:

A. Makes any warranty or representation, exprassed or implied, with respect to the accuracy,
completeness, or usefulness of the information contained in this report, or that the use of
any information, cpparatus, method, or process disclosed in this report may not infringe
privately owned rights; or

B. Assumes any liabilities with respect to the use of, or for damages resulting from the use of
any informotion, apparatus, method, or process disclosed in this report.

As used in the above, '‘person acting on behalf of the Commission® includes any employee or

contractar of the Commission, or employee of such contractor, to the extent thoat such employas

or contractor of the Commission, or employes of such contractor prepares, disseminates, or
provides access to, any informotion pursvant to his amployment or contract with the Commission,

or his employment with such contractor,

 

 
ORNL-TM-2335

Contract No. W-7405-eng-26

REACTOR CHEMISTRY DIVISION

SOLUBILITY OF CERIUM TRIFLUORIDE IN MOLTEN MIXTURES OF
LiF, BeF,, AND ThF,

Judy A. Fredricksen’} L. O. Gilpatrick,
C. J. Barton

JANUARY 1969

*Summer ORAU Participant from St. Cloud State College,
St. Cloud, Minnesota

OAK RIDGE NATIONAL LABORATORY
Oak Ridge, Tennessee

operated by

UNION CARBIDE CORPORATION
for the

U.S. ATOMIC ENERGY COMMISSION

LEGAL NOTICE

This report was prepared as an account of Government sponsored work. Neither the United
States, nor the Commission, nor any person acting on behaif of the Commission:

A. Makes any warranty or representation, expressed or implied, with respect to the accu-
racy, compleieness, or usefulness of the information contained in thig report, or that the use
of any information, apparatus, method, or process disclosed in this Teport may not infringe
privately owned rights; or

B, Assumes any liabilities with respect to the uge of, or for damages resulting from the
use of any information, apparatus, method, or process disclosed in this report,

Ag used in the above, ‘‘person acting on behall of the Commission®’ includes any em- B g rme B 2R EUDR L“ Tt JRALTRER
ployee or contractor of the Commission, or employee of such contractor, to the extent that SARTRIEISIR O VLAY T D ttE s U P
such employee of contractor of the Commission, or employee of such confracter prepares, " W
disseminates, or provides access to, any information pursuant to his empioyment or contract
with the Commission, or his employment with such centractor.

,,,,,,,,,,,
iii

CONTENTS

Abstract

Introduction
Equipment.

Materials.

Procedure.

Results and Discussion

References.

Page

 

21
SOLUBILITY OF CERIUM TRIFLUORIDE IN MOLTEN MIXTURES OF
LiF, BeF,, AND ThF,

 

 

Judy A. Fredricksen,* L. O. Gilpatrick,
C. J. Barton

ABSTRACT

The solubility of CeF,; was determined at various
temperatures in six mixtures of LiF, BeF,, ThF, of
the type that may be used to fuel a molten salt breeder
reactor. Comparison of earlier data on the solu-
bility of PuF; and CeF; in fluoride solvents makes
it possible to predict that the solubility of PuF,
in single-region fuel compositions at reactor
operating temperatures will be more than adequate.
The solubility data as a function of solvent compo-
sition were best correlated by a model that assumes
BeF, to be complexed as the BeF,?~ ion and ThF, as
the ThF !~ ion.

INTRODUCTION
Studies performed earlier at the Oak Ridge National
Laboratory demonstrated the solubility of PuF, in certain
molten fluoride solvents,1 but no data are available on the
solubility of PuF,; in single-fluid reactor fuel containing a
high concentration of ThF,. Previous data indicated that the

solubility would probably be adequate at proposed reactor

 

X
Summer ORAU Participant from St. Cloud State College,

St. Cloud, Minnesota.
operating temperatures. To verify this belief, the most
obvious approach would be direct measurement of PuF; solu-
bility in molten fluoride salts of interest, but we have chosen
to study the solubility of anothexr trivalent fluoride, CeF,,
because of its similar behavior and simpler handling. There

is evidence indicating that PuF; and CeF; are quite similar in

253 A thorough

their solubility behavior in fluoride melts.
study of the effect on the solubility of CeF,; of varying the
concentrations of LiF, BeF, and ThF, in melts will indicate
the probable solubility of PuF; in such melts. This investi-
gation may be followed by limited determinations of PuF, solu-
bility to confirm predictions based on the CeF,; investigation.
The chemical feasibility of fueling molten salt reactors with
PuF,; has been considered in another report.4
This report gives the results obtained to date in an

investigation on the solubility of CeF; in mixed LiF, BeF, and

ThF, molten fluoride solvents.

EQUIPMENT

The reaction vessel in which the solubility measurements
were made was a welded cylindrical nickel container with an
internal diameter of 13 in., a depth of 6%+ in., and a wall
thickness of 1/8 in. A seven-inch section of }-in. I.D.
nickel pipe was welded to the 1lid and was closed at the top
with a stainless steel ball valve having an internal clearance
of & in. This cooling and loading stem was also equipped with

a 1/4-in. gas discharge port welded near its upper end. An
additional opening in the 1lid accommodated a thermocouple well
of 1/4-in. thin wall (10 mil) nickel tubing closed at the lower
end, which extended to within 1/8 in. of the bottom. The
remaining lid opening held a 1/4-in. nickel dip leg of heavy
wall (35 mil) nickel tubing extending to within 1/4 in. of the
vessel bottom to facilitate agitation and purification of the
melt by admitting gases beneath the melt surface.

The vessel was mounted vertically in a 3-in., 1400-watt
electric tube furnace whose temperature was regulated by means
of a chromel-alumel thermocouple placed between the furnace
wall and the vessel and a high-sensitivity bucking circuit
controller.

Melt temperatures were determined by a second chromel-
alumel thermocouple located in the thermocouple well surrounded
by the melt. An ice bath, a standard cell, and a Leeds and
Northrup type K-2 potentiometer were used to measure the E.M.F.
in this measuring circuit. Temperatures were deduced from
standard tables of temperature versus E.M.F.

Copper filter sticks were constructed from 3/8-~in. diameter
sintered disk fritts 1/8-in. thick with a nominal pore size of
0.0004 in. These were welded into sections of 3/8-in. 0.D.
tubing 1/2-in. long. At the opposite end, this tube was reduced
in diameter and welded to a 20-in. length of 1/8-in. 0.D.
tubing. These tubes were slipped through a Teflon gland made
to fit a 1/2-in. Swagelok tubing connector and compressed by a

standard connector collar. This gland formed a vacuum tight
seal around the 1/8-in. filter tube but it allowed movement
of the filter through the gland which was fitted to the top
end of the ball valve. Sufficient space was provided between
the closed ball of the valve and the gland to accommodate the
filter unit for evacuation and flushing with helium prior to
admitting it to the clean (oxide free) melt. A piece of soft
rubber tubing which fitted over the free end of the filter
stick could be connected to either a vacuum pump or a helium
source. A manifold system consisting of valves, pressure
gages, and flow meters controlled admission of helium, hydrogen,
HF or application of vacuum to the apparatus.

Samples containing !'4%*Ce tracer were analyzed using a
256-channel or 400-channel analyzer at fixed geometry with a
3 x 3 in. NalI, thallium activated crystal. Sample preparation
and weighing was done in a hood equipped with a dust contain-

ment glove box.

MATERIALS

Some of the compositions used in these studies were supplied
by J. H. Shaffer and F. A. Doss of ORNL. Mixtures of LiF, BeF,,
and ThF, (72-16-12 and 68-20-12 mole %) were used as received
as was a mixture of LiF and ThF, (73-27 mole %) . The (72.7-
4.8-22.5) mixture was prepared by adding 53 g of (72-16-12) to
198 g of the 73-27 residue left in the vessel after previous
solubility determinations. Likewise a mixture calculated to
have the composition (72.3-11.0-16.7) was prepared by adding

195.5 g of (72-16-12) to 225.1 g of (73.1-4.8-22.4) remaining
at the end of a series of measurements. A mixture having the
composition (67.8-25.2-7.0) was prepared by mixing 94.7 g of
66 LiF - 34 BeF, with 102.1 g of the 73-27 preparation.

Ten millicuries of 1%4%4Ce in the form of an aqueous HCl
solution was secured from the Isotopes Division at ORNL. This
was mixed with a solution containing 308 g of CeCl, x H,0.*
The resulting solution was heated to 9OOC and digested with
214 g of NH,F.HF** dissolved in 1000 ml of H,0, which yielded
a homogeneous precipitate of CeF; containing the radioisotope.
This precipitate was washed with distilled water four times
and centrifuged before drying at 110°C for 24 hours.

Commercial hydrogen was purified by passage through a
Deoxo unit, a magnesium perchlorate drying tube, and a liquid
N, trap. Anhydrous HF (99.9%), was used from the cylinder as
received without purification. Commercial helium was purified
by passage through an Ascarite trap, a magnesium perchlorate

trap, and a charcoal trap at liquid N, temperature.

PROCEDURE
Helium leak testing was done at room temperature prior to
loading the unit until a vacuum of at least 74 microns was
secured. A weighed amcunt of fuel salt, usually about 250
grams, and more than the amount of CeF; expected to dissolve

at the maximum temperature were added to the vessel through

 

* A. D. MacKay, Inc., C.P. grade.

* % , ‘
Baker and Adamson, technical grade.
the open ball valve by means of a long-necked funnel. The
apparatus was then connected to the manifold system. A
heated sodium fluoride trap was placed at the outlet to
preveat HF from escaping into the hood. This was followed by
a bubbler to indicate when gas was flowing through the system.

Purification was carried out at about 625°C by treating
the melt with gaseous HF (20 ml/min), H, (100 ml/min), and
helium (100 ml/min) for at least three hours. Hydrogen
fluoride eliminated any products of hydrolysis resulting from
adsorbed water on the surface of the fuel salt by converting
them to fluorides. The hydrogen helped to minimize the cor-
rosiveness of the HF by reducing any NiF, produced to Ni while
the helium served as a carrier gas. Next, the melt was
subjected to two hours of hydrogen (100 ml/min) -— helium
(100 ml/min) treatment to complete the reduction of any NiF,
formed.

Hydrogen and helium flow rates were measured by rotameters
calibrated with a "Bubble-O-Meter." The hydrogen fluoride flow
rate was measured by passing the gas mixture through a measured
volume of 0.1 M KOH solution using phenolphthalein as an
indicator and a stop watch to determine the time necessary
for neutralization.

The mixture in the apparatus was allowed to equilibrate
for one hour starting at the highest sampling temperature
while agitation was maintained by a slow helium flow of 30 ml

per minute. Each melt, with an excess of CeF;, formed a
saturated solution at the selected temperature which was then
sampled to determine the concentration of CeF; in the filtered
melt. Sampling was performed by assembling the filter stick,
after polishing with steel wool to remove the oxide coating,
and the gland above the closed ball valve. This area was
sealed by tightening the threaded collar around the Teflon
gland, and a vacuum was applied followed by flushing with
helium to remove air. This flush was repeated before the ball
valve was opened and the filter was inserted to within 1/2-in.
of the vessel bottom. A small flow of helium was maintained
through the filter stick while it was being inserted and
submerged. Five or ten minutes was allowed for the filter to
reach the melt temperature before the helium flow was stopped
and a vacuum was applied to the stem. The salt froze in the
1/8-in. diameter cold stem of the filter stick. Samples were
withdrawn slowly to protect the Teflon gland from over heating.
After closing the ball valve, the filter stick was removed by
disassembling the gland and compression collar. It was then
cut open and emptied in the glove box where the melt samples
were ground and 50 mg f 3 mg was weighed from each filter for
counting and one gram for wet chemical analysis.

The 50 mg portions of ground salt were weighed and placed
in plastic vials 1l-in. in diameter and 2-in. high. Six samples
were drawn at 40°C intervals ending at about ZOOC above the
melting point of the salt compositions. Seven channels

centering around the most energetic 4 disintegration at
0.124 M.E.V. were integrated during the counting which was
done mostly for one minute intervals.

Analyzing the samples radiochemically involved preparing
standard samples made for each molten salt mixture consisting
of 50 mg of solvent (+ 5%) plus varying amounts of accurately
weighed CeF, tracer salt. A blank was also prepared which
contained only the solvent which was used to determine the
value to be subtracted from the total count to correct for
the gamma activity of thorium daughter products. The net
counting rate obtained for each standard was plotted on a
linear scale against milligrams of labeled cerium fluoride.
These calibration data made it possible to determine the
number of milligrams of CeF; present in each sample from the
count rate. From these values we calculated the mole percent
of cerium fluoride present in each molten salt mixture at
the various temperatures. No adjustment was made for radio-
active decay since the half life of '*%*Ce is 285 days and
all counting for a given set of samples, including calibra-

tions, was performed in sequence on a single day.

RESULTS AND DISCUSSION
The data obtained are plotted in Figs. 1-6, inclusive.
Both radiochemical and wet chemical analysis are shown in these
plots. In general, the agreement between the two methods of
analysis is considered quite satisfactory. In some cases,
comparison of the data required rechecking the wet chemical

analyses and, in others, re-examination of the radiochemical
ORNL-DWG 68-12064
TEMPERATURE (°C)

 

 

 

 

 

 

 

 

 

700 600
10 T | T
8
5 O RADIOCHEMICAL ANALYSIS ]
e WET CHEMICAL ANALYSIS
4 s ~ ;

 

 

 

 

~.

 

 

 

 

CeFy (mole %)

 

 

0.6

 

 

0.4

 

 

0.2

 

 

 

 

 

 

0.1 '
1.0 1.1 1.2

1000/ (o)

Fig. 1. Solubility of CeF; in LiF-BeF,-ThF, (72-16-12 mole %).
10

ORNL-DWG 68-12063
TEMPERATURE (°C)

800 700 600
10 I I

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

6 5 —

5

®

4
52 \Q
Q
o
£ \\\\
- 3
u® \\
3 o RADIOCHEMICAL ANALYSIS 0\

e WET CHEMICAL ANALYSIS o \
\
\
! \

2

1 Y

0.9 1.0 1.1 1.2

1ooo/r(°K)

Fig. 2. Solubility of CeF; in LiF-ThF, (73-27 mole %).
11

ORNL-DWG 68—42065
TEMPERATURE (°C)
800 700 6C0

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

{0 I ]
'\
N\
8 N
\ O
2 \
© ®
° \
© \
: N
B2
v 4 .
©
E
L
QO
Q .\
3 N,
0 RADIOCHEMICAL ANALYSIS
® WET CHEMICAL ANALYSIS
“
\
N\
> \
1
0.9 {.0 {1 t.2

1000/, 1

Fig. 3. Solubility of CeF; in LiF-BeF,-ThFy (72.7-4.8-22.5
mole %) .
12

ORNL-DWG 68-12066
TEMPERATURE (°C)
800 700 600
I T

 

 

 

 

 

o RADIOCHEMICAL ANALYSIS
e WET CHEMICAL ANALYSIS

 

 

 

 

CeFy {mole %)
®

 

 

 

 

 

 

0.8 1.0 1.1 1.2
1000/ ek)

Fig. 4. Solubility of CeF, in LiF-BeF,-ThF, (68-20-12 mole %).
13

ORNL~DWG 68-12067
TEMPERATURE (°C)

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

800 700 600
10
l l |
9 _
8
7
\\
6
N\
N\
N\
5 \\
N\
\l
© N
5 .
@
O
E
u-l"')
® 3
O
AN
\\\g
2 \\
N
o RADIOCHEMICAL ANALYSIS \
e WET CHEMICAL ANALYSIS
{ :
0% 10 11 : 1.2

1990

Fig. 5. Solubility of CeF, in LiF-BeF,-ThF, (72.3-11.0-16.7
mole %) .
CeFz (mole %)

Fig. 6.

14

ORNL-DWG 68 - 12068

TEMPERATURE (°C)

700
I

600

 

 

 

o RADIOCHEMICAL ANALYSIS
e WET CHEMICAL ANALYSIS |

 

 

 

 

 

 

  

 

 

 

0.9

Solubility of CeF,

mole %) .

1.0

1.1
1000 /7 s

in LiF-BeF,-ThF,

(67.8-25.2-7.0
15

calibration values. It is apparent in Figs. 3, 5, and 6 that
insufficient CeF, was present in the system to saturate the
melts at the highest temperatures. The data are summarized
in Table 1 together with heats of solution calculated from

the relation

SZ — AI-I(TZ'—TI)
log’sT =~ 2.303 RT, T,

where S, is the solubility (in mole %) at the higher tempera-
ture and S; 1is the corresponding value at the lower temperature.
The heats of solution are in approximately the same range as
those reported1 for solutions of PuF; in various fluoride
solvents (12,000 to 16,800 cal per mole).

The solubility data obtained in this investigation are
very reassuring in respect to the potential use of PuF; as
the fissionable species in single-region fuel compositions.
The lowest solubility observed at 600°C was 1.05 mole %. A
comparison of PuF; solubility data1 with similar values
reported2 for CeF; in Fig. 7 indicates that the solubility
of PuF, at 600° may be less than 1.0 mole % but will almost
certainly exceed the few tenths mole % value required to fuel
a single region breeder reactor.

Bredig has Suggested5 that the ""free fluoride" content of
liquid mixtures of LiF, BeF,, and ThF, can be calculated from
the following relation in terms of mole %:

Free fluoride = LiF - 2(BeF,) - 3(ThF,)

This relation is based on the assumption that LiF is complexed
16

Table 1. Solubility and Heat of Solution of CeFsj

in Mixtures of LiF, BeF,, and ThFy

 

 

 

Salt Composition CeF3 Solubility Heat of Solution
(mole %) (mole %) (cal per mole)

LiF BeF,  Thfy 600°c  800°C

72 16 12 1.6 5.5 11,500
73 0 27 2.6 9.0 11,560
72.7 4,8 22.5 2.4 7.9 11,100
68 20 12 1.35 6.0 13,890
72.3 11.0 16.7 2.1 6.3 10,230
67.8 25.2 7.0 1.05 5.0 14,530

 

 

 
17

ORNL-DWG 68-5997

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

1.8
16 |-
1.4
R
@ 42
o
£
0
CeF, —650°
2 . \ s 650
= PUF, ~ 650°
) ;'3
L o ®
- 1\
Z X 7.
M A o
L 0.8 }\ \\( / CeFz—600
a
@ /
O ®
Lm0 ‘\ \ ,PUF3—SOO
& 06 ® \ .
\/ /
®
®°  CeF,~550°
3
\,// PA )
04 9/ PuF,~550
. ./
\.___/
0.2
0
10 20 30 40 50 60

BeF, IN SOLVENT (mole %)

Fig. 7. Comparison of CeF,; and PuF; Solubility in LiF-BeF,
Solvents.
18

as Li,BeF, and Li; ThF, in the liquid state. It is interesting
to test this concept with the CeF; solubility data reported
here. The resulting graph (Fig. 8) shows a rather poor
correlation based on this relationship. A somewhat better
correlation, shown in Fig. 9, results from the assumption
that BeF, is complexed in the liquid state as Li,BeF, and
ThF, as LiThFy;. The latter assumption has a rather shaky
basis since the published phase diagram6 for the system
LiF-ThF, indicates that the 1:1 compound (as it is now known
to be7) melts incongruently. The only defense for this
assumption is that five of the six compositions tested to

date show solubility data that correlate on this basis.

REFERENCES
1. C. J. Barton, J. Phys. Chem. 64, 306 {(1960).
2. W. T. Ward, R. A. Strehlow, W. R. Grimes, and
G. M. Watsom, J. Chem. Eng. Data 5, 2 (1960).
3. C. J. Barton, Memo to P. R. Kasten, June 4, 1968,
MSR 68-88.

4. R. E. Thoma, Chemical Feasibility of Fueling Molten

 

Salt Reactors with PuF,, ORNL-TM-2256, June 20, 1968.

 

5. M. A. Bredig, Memo to W. R. Grimes, April 26, 1968,
MSR 68-75.
6. R. E. Thoma et al, J. Phys. Chem. 63, 1267 (1959).

7. G. Brunton, Acta Cryst. 31(5), 814 (1966).
19

ORNL-DWG 68-12069

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

10.0 T T T
o 73LiF-27ThF,
9.0 ¢ 68 LiF-20BeF,~12ThF, —
N ® 67.8LiF-25.2Bef,- 7.0 ThF,
8.0 N & 72.3LiF-1.0 BeF,-16.7 ThF,
\4{ © 72 LiF-16BeF,-12 ThF,
\ | 4 72.7LiF-4.8BeF,-22.5ThF,
7.0 \ , .
\ |
~ 800°C
2 6.0 \ //&fifi‘\\
2 Aoy N |
=, 5.0 >y So
L N
@ M
" 40 N
| \ S T700°C
\ / \
3.0 "‘\ \‘\ v
(L-—-.."‘\'f'"}./
I\‘
2.0 \\ Lar— 600°C
\\ ,////4 ~\\\\\$
¢
1.0 b= Mo
0

FREE LiF (mole %)

Fig. 8. Solubility of CeF; As A Function of Free LiF Assuming
Li,BeF; and Li;ThF, In Liquid.
20

ORNL-DWG 68-42070

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

© T3 LiF-27ThF,
. & 68LiIF-20 BeF2—12 ThF4

e 67 8LiIF-25.2 BeF2—7.O Th Fq
L A& 72 .3LiF-110 BeF2—16.? ThF4

¢ 72 LiF-16BeF>- 12 ThF, o
A 72.7TLIF-4.8 BeFZ— 22.5 ThF4 /|

A/
/,
. /
/
N sooec_| € 1
g ‘ /////A///,
——— ‘;r . e /’
o 700°C_%
—-——M
- | o5
. L

. 600°C_—
‘ ./. |

l i

 

 

 

 

 

5 10 15 20 25 30 35 40 45
FREE LiF (mole %)

Fig. 9. Solubility of CeF, As A Function of Free LiF Assuming
Li,BeF, and LiThF; in Liquid.
21

REFERENCES

C. J. Barton, J. Phys. Chem. 64, 306 (1960) .

wW. T. Ward, R. A. Strehlow, W. R. Grimes, and G. W.
Watson, J. Chem. Eng. Data 5, 2 (1960).

C. J. Barton, Memo to P. R. Kasten, June 4, 1968,
MSR 68-88.

R. E. Thoma, Chemical Feasibility of Fueling Molten
Salt Reactors with PuF;, ORNL-TM-2256, June 20, 19638.

 

 

M. A. Bredig, Memo to W. R. Grimes, April 26, 1968,
MSR 68-75.

R. E. Thoma et al, J. Phys. Chem. 63, 1267 (1959).

G. D. Brunton, Acta Cryst. 21(5), 814 (1966).
23

ORNL~-TM-2335

INTERNAL DISTRTIBUTION

1. R. K. Adams A7. D. R. Cuneo

2. G. M. Adamson 58. J. M. Dale

3. R. G. Affel 59, D. G. Davis

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5. J. L. Anderson 61, J. H. DeVan

6. R. F. Apple 62. S. J. Ditto

7. C. F. Baes 63. A. S. Dworkin

8. J. M. Baker 64. I. T. Dudley

9. S. J. Ball 65, D. A, Dyslin
10. €. E. Bamberger 66, W. P. Eatherly
11-21.. C. J. Bartéon 67. J. R. Engel

22. H. F. Bauman 68. E. P. Epler

23. S. E, Beall 69. D. E. Ferguson
24. R. L. Beatty 70, L. M. Ferris
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27. C. E, Bettis 82. H. A. Friedman
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52. W. H. Cook 107, H. W. Hoffman
53, L. T. Corbin 108. D. X. Holmes
54. B. Cox 109, P. P. Holz

55. J. L. Crowley 110, R. W. Horton
56. F. L. Culler 111, T. L. Hudson
112.
113.
114.
115.
116.
117.
118.
119.
120.
121.
122.
123.
124.
125.
126.
127.
128.
129.
130.
131].
132.
133.
134.
135.
136.
137.
138.
139.
140.

141

142.
143.
144,
145.
146.
147.
148.
149.
150.
151.
152.
153.
154,
155.
156.
157.
158.
159.
160.
161.
1l62.
163.

.

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24

Kasten
Kedl
Keller
Kelley
Kelly
Kennedy
Kerlin
Kerr
Kirslis
Koger
Krakoviak
Kress
Krewson
Lamb

Lane
Lawrence
Lin
Lindauer
Litman
Llewellyn
Long
Lundin
Lyon
Macklin
MacPherson
MacPherson
Mailen
Manning
Martin
Mauney

Claln

McClung
McCoy
McDuffie
McGlothlan
McHargue
McNeese
McWherter
Metz
Meyer
Moore
Moulton
Mueller
Nelms
Nichols
Nicholson
Nogueira
Oakes

Patrlarca

M.

Perry

164.
165.
166.
167.
168.
169.
170.
171.
172.
173.
174.
175.
176.
177.
178.

179

180.
181.
182.
183.
184.
185.
186.
187.
188.
189.
190.
191.
192.
193.
194.
195.
196.
197.
198.
199.
200.
201.
202.
203.
204.
205,
206.
207.
208.
209.
210.
211.
212.
213.
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215.

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Pickel
Piper
Prince
Ragan
Redford
chardson
Robbins
Robertson
Robinson
Roller
Romberger
Rosenthal
Ross
Savage
Schaffer
Schilling
p Scott
Scott
Seagren
Sessions
Shaffer
Sides
Skinner
Slaughter
Smith
Smith
Smith
Smith
Smith

p1ewak

Steffy
Stoddard
Stone
Strehlow
Tallackson
Taylor
erry
Thoma
Thomason
Toth
Trauger
Watson
Watts
Weaver
Webster
Weinberg
Weir
Werner
West
Whatley
White
Wilson
216.
217.
218.
219.
220.
221-222.
223-224.
225-239.
240.

241-242.
243.
244 .
245,
246 .
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256-270.

25

Gale Young

H. C. Young

J. P. Young

E. L. Youngblood

F. C. Zapp

Central Research Library

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