ORNL-TM-2170.txt

CHHEED MARTIN ENERGY RESEARCH LIBRARIES

LO
IEER AT 150

| 3 445L 0513008 & ‘'IONAL LABORATORY

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

— ——operated by
UNION CARBIDE CORPORATION
NUCLEAR DiVISION o “RB'DE
for the oDt e R e

N
DOCUMENT &0 L EOTION

U.S. ATOMIC ENERGY COMMISSION
ORNL- TM- 2170

 

HOT-CELL STUDIES OF THE FLUIDIZED-BED FLUORIDE VOLATILITY PROCESS
FOR RECOVERING URANIUM AND PLUTONIUM FROM SPENT UO,, FUELS

J. C. Mailenand G. |. Cathers

bAK RIDGE NATIONAL
CENTRAL RESEARC
DOCUMENT COL
LIBRARY LO

DO NOT TRANSFER TO A

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document, send BT

and the library will arra
UECN-796% 1

{3 3-671 f

 

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

bbb . LEGAL NOTICE — — S

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

nor the Commission, nor any person dacting on behalf of the Commission:

A. Makes any warranty or representaticn, expressed or implied, with respect to the accuracy,
completeness, or usefulness of the information contained in this report, or that the use of |
any infermation, aopparatus, methed, 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 damoges resulting from the use of
any information, apparatus, methed, or process disclesed in this report.

As used in the cbeve, ““person acting on behalf of the Commissien®’ includes any employee or

contractor of the Commission, or employee of such cantractor, to the extent that such employee

or contractor of the Commission, or employee of such contractor prepares, disseminures, or
provides access to, any information pursuant to his employment or controct with the Commission,

or his employment with such contractor. '

 

   
ORNL~ TM- 2170
Contract No. W-Th05-eng-26

CHEMICAL TECHNCILOGY DIVISION

Chemical Development Section B

HOT-CELL STUDIES OF THE FLUIDIZED-BED FLUORIDE VOIATILITY PROCESS
FOR RECOVERING URANIUM AND PLUTONIUM FROM SPENT UO2 FUELS

J. C. Mailen and G. I. Cathers

APRIL 1969

OAK RIDGE NATIONAL LABORATCRY
Oak Ridge, Tennessee
operated by
UNTON CARBIDE CORPORATION
for the
U.S. ATOMIC ENERGY COMMISSION

ENEPGY RESEARCH LIBRARIES

T

 

 

 

 

|

3 yy5kL 0513008 &

 

 

 

 

 

 

 

 

 

 

 

 

 

 

b
CONTENTS
Abstract
1. Introduction .
2. Hxperimental .
2.1 Equipment Used . . . ¢ « « « o« « « .
2.2 Sampling Procedure
2.3 Experimental Materials . . . . . . .
3. Results and Discussion « . « « « « « + + .
3.1 Oxidation of Fuel . . . . . . . .
3.2 Volatilization of Uranium with BrF5
3.3 Desorption of Uranium .
3.4 Volatilization of PuF6 with Fluorine
3.5 Recovery of Plutonium from Nal Trap
. Conclusions
5. References

10

10

10

12

. 21

. 21

. 29

29
30
HOT-CELL STUDIES OF THE FLUIDIZED-BED FLUCRIDE VOIATILITY PROCESS
POR RECOVERING URANIUM AND PLUTONTUM FROM SPENT UO_. FUELS

 

 

Jd. C, Mgilern and G. T. Cathers

ABSTRACT

Bench-scale experiments with UO2 that had been irra-
diated to a burnup of 34,000 Mwd/metric ton and cooled for
two years were performed, using a 0.94-in.-ID fluidized-
bed resctor. The objectives of these experiments were to
test NaF at 400°C for use as a trap Tor volatile fission
product fluorides, to test MgF2 for use as a Lrap Tor nep-
tunium and technetium fluorides, to test NaF at 550°C for
use as a trap Tor sorbing PuF6 and separating it from ru-
thenium, to study the behavior of neptunium, and to deter-

mine the fate of tritium.

In these studies the U0, wes first oxidized with 20%
02--80% N, at h50°C, to form U308; this was then btreated
with BrF5~N2 mixtures (5 to 10% BrF5) at 300°C to form
UF6 and volatllize the uranium and most of the ruthenium,
molybdenun, and techonetium fluorides; finally, treatment
with fluorine at 300 Lo 500°C was used to Tluorinate and
volatilize the plutonium as PuFé. In some runs, BrI, was

3

used for a finsl cleanup of uranium after the BrF5 tfeat—
ment. Plutonium was separated from the fluorine stream,
by irreversible sorption on NaF, in a trap at lemperatures
above 500°C. Uranlium hexafluoride was purified by passage
through a 400°C WaF bed and by sorption on, and desorption
from, Nab'.

A ruthenium decontamination factor of 2000 was ob-
tained by using a 400°C NaF ted and a residence time of

15 sec; cosorption of ruthenium in the plutonium Utrap
was minimized by operating it at 550 to 600°C. Of the
syitium in the fuel, about 95% was liberated during the
heatup of the fuel to 450°C and during the oxidation; the

other 5% was liberated during the BrF_ step.
J

1. INTRODUCTION

Hot-cell tests of the fluldized-bed Tluoride volatility process
were made at Oak Ridge National Iaboratory in support of the proposed
Tuidized-Bed Volatility Pilot Plant.® These studies were designed to
explore The chemical behavior of various fission products, using high-
burnup tuel, ana tc evaluate methods Tor decontaminating the uranium

and plutonium products. Opecifically, we attempted to do the Tollowing:

1. test NaF at LOC°C Tor its effectiveness in removing vclatile
fission products,

2. test MgFP at 100°C for use 22 & neptunium and technetium trap,

2. test NalF for use as a plutonium trap, particularly regarding
cosorpvion of ruthenium,

4. examine the behavior of ueptunium, and

5. determine the fate of tritium.

The results of these tests and examinations, along with significant
observations made in the course of the work, are presented in this

report.

Acknowledgmente. — The authors wish to recognize the fine work
acne oy the Analytical Chemistry Division in the analysis of the hot
samples, and that of J. H. Goode Tor his analysis of the tritium and
plutorium content of the fuel. We were assisted in the initial cold
teating ol the equipment by T. E. Crabtree; the hot-cell work was

o

performed with fthe assistance of L. A. Byrd.

 

*Design and construction efforts involving the Fluidized-Bed
VolaTility Pilot Plant, which was scheduled for installation in
s1de. 3019, were terminsted in the 211 of 1967 zccording to a direciive
pued oy Lhe USAEC,

 
L

2. HEXPERIMENTAT

2.1 HEoulpment Used

Because space was limited the hoft-cell tests were done with small
equipment. The fluidized-bed reactor, which was made of 1-in.-0D
nickel pipe, had a2 2-in.-0D disengaging section. Except for the cold
trap and the Na¥ trap for plutonium sorption, the variocus traps con-

sisted of 1- or 2-in.-0D nickel tubes.

The fluidized-bed veactor is shown in Fig. 1. The bed was
supported in the reactor by a ball check valve. The temperature of
the fluidized section was monitored by an external thermccouple in a
well that was welded to the side of the reactor. Heat was supplled to
the fluidized-bed portion of the reactor by a clamshell heater. The
temperature of the disengaging secltion wasg monitored by an external
thermocouple. Calibration of this thermocouple against an internal
thermocouple indicated that the temperature cf the gas in the disengaging
section was about 30°C higher than that of the wall. The disengaging
section was heated by means of a wrappling of asbestos-coeoated resistance
wire (Cerro Corp. "Rockbestos') thermally insulated with Ssuereisen.
The filter at the top of the disengaging section was periodically blown
back by a pulse of 5- to 10-psig nitrogen. The coaxial tube arrangement
shown in Fig. 1 created sufficient restricticn in the flow out of the
bed to ensure that more than half of the blowback pulse passed through
the Tilter. This arrangement eliminzated the use of valves, which were

known to require frequent maintenance.

Figure 2 shows the flange-filter assembly that was used on the
fluidized-bed reactor and on all traps except the cold trap and the
Na¥ trap for plutonium. TIn this design, the Teflon O-ring acts to
seal the Tlanges and to seal in the Tilter. The presence of these
filters at the top of each trap prevented significant transfer of dust

vetween traps. The Tilters were replaced after each run.

The traps (except the cold trap and the plutonium trap) were

heated with resistance wire wrappings and were insulated with Sauereisen.
FILTER
- BLOWBACK
l‘ PULSE

éifl()D

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SEE FLANGE-FILTER
ASSEMBLY DRAWING

GAS

TREATMENT

a in. 0.0,

32-mil WAL L

Schematic Dliagram

 

 

 

 

ORNL. DWGC. ©9-85
FILTER
BLOWEACK
PULSE
SEE
DETAHfE”\\& Y
; ngfi _TO GAS
g T TREATMEMT
l\ /.’
\\ //
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<THERMOCOUPLE
R e
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-
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4
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N\
e MONEL BALL

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SEE ; /2 TO 3/4 in.
A » .
DETAIL "A" ~TE DIAM

of tne C.94-1n.~-1D Fluidized-Bed Reactor
-

 

1.
4m.

ORNL DWG 69-88

FLANGES TIGHTENED
BY THREE, 3/8-in,
BOLTS ON 120°

X CENTERS
o \

 

 

Tl 700

 

 

 

r‘

A

(

 

 

 

Z

 

 

 

3/32-in. THICK

 

TEFLON O-RING
/2 9/16-in. 1. D.,
L)

 

 

 

.

- |

~-HUYCK SINTERED

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

3 NICKEL FIBER
(e — 27 i7" n5i5¢ 80 mil. THICK,
ro.oezin. | 2 9/16-in. 0. D.
1
4 7 7 =/
0.625in. //f/ —=
Y \ e / —
|
4 4
2 i

 

 

Fig. 2.

4in.

 

 

otandard Flange-Filter Assembly.
The bottom plates were recessed within the heated tubes tTo prevent a
temperature decrease at the bottom of the trap. In each o7 these traps,
the gag entered the trap at the bottom znd exited at the top through =
flarge-[ilter sssemoly.

The cold trap, which was used to collect the UF6 product, consisted

of 2 6-in.~long, 2-in.-0D nickel tube Titted with a baffle that Torced

the gas to circulate to within 2 in. of the bottom. The Trap was cooled

by Immersicn in dry ice-~trichlorcetiylene.

In the Tirst four hot-cell tests, the plutenium trap consisted of
a straight tupe having a thermocouple well that entered the side about
hailfway down the tube; here, the two Nal' beds were supported on each
side ol the therymocouple well. The disgsdvantsge of this type of trap
was the large =emperature differential (50 to 100°C) across the section
of Nel¥ on the g=s inlet side. The NaF trap used fTo scorb plutonium in
the most recent tests is shown in Fig. 3. The double-wall design
resulted in a very small temperature gradlient in The ianer tube. Two
2.5-g portions of 12- Cto 20-mesh Nal', separsted by a plug of 3-mil
nickel wire, were ingerted Into this inner bube. The highest termpera-
ture cccurred at the bottom of the irner tube. The decreases in tem-
perature over the first and second sectlions were about 1°C and about
4°C, respectively. Thus, this trap could be operated with an essentially

constant sorption temperature; 1t was hested with = clamshell furnace.

Unheated 1/4-in.-0D Kel-F lines served to connect the fluidized-
bed reactor, gas suppliecs, and the various traps. No valves were used

inslide the cell except on the uranium product cold trap.

O"f-gas from the process was pasced through the scrubber shown

in Fig. 4. The BrFS and fluorine streams were scrubbed with 2 N

KOH--0.2 N KT solution in 100% excecs, =nd the gss resulting from the

foue]
oxidztlon step was scrubbed with water. Representative sarmulec of
the scrubber offluent were withdrawn asutomatically by means of the
solercid velve and Limer locaied at the bottom of The column.
Gee Tlowe into the cell were moritored with differentisl prossure
1

transmitters {Foxboro 15A-152). Nitrogen, oxyzen, and Muorine were
 

 

 

 

 

ORNL DWG 69-9i

 

 

 

 

 

 

 

 

 

 

 

 

 

 

—iind 12 in. leg——
THERMOCOUPLE
WELL
%in. Ni TUBE
3 r 1 ’/_
- GAS
SUPPORT INLET
g DISC
1. [
2 In.
5in
3~ in
_— 8 HOLES, 1/32 in.
DIAM, DRILLED CLOSE
, / TO BOTTOM OF TUBE
= in.
? g_qgfl/
; - {
o | |, ——~

Fig. 3. Plutonium Trep Used in Most Recent Tests.
ORNL DWG 62-8¢

PROCESS GAS 2 N KOH
CONTAINING ——»—1[—4~ 0.2 MK
BrFg OR Fp SOLUTION
1-in-SWAGELOK

1-in-0.0. BY——""|
rfi-Lone | r/_,, CONNECTOR

ALUNDUM TUBE [
. /1—in.-»o,0. ay 2-f1-LONG

 

 

    

 

 

 

 

 

 

 

 

 

 

 

 

 

To | P STAINLESS STEEL TUBE
sggggggg; REACTOR COLUMN PACKED
47 WITH FUSED ALUMINA
f + 1-in-SWAGELOK
wi“* CONNECTOR
TIMER
2004,
SOLENOID
VALVE
T0 TO
DISFOSAL SAMPLE
CONTAINER

Fig. k. Tluorine and BrF5 Disposal Apparatus Used in Hot-Cell

Experiments.
piped through ambient-temperature tubing Into the cell. Bromine
pentafluoride gas was generated by heating a cylinder of liquid BrFs to
shout 50°C and passing it through tubing and differential pressure
transmitters heated above this temperature. Before entering the cell,
the BrF5 zas was diluted with nitrogen to eliminate the necessity of

heating the lines inside the cell. Bromine trifluoride was produced

al the dinlet of the fluidized-bed reactor by mixing appropriaste amounts

of bromine =and Br¥F_. Bromine was generated by passing nitrogen through

2

2 bromine bubbler maintained at 0°C.

2.2 Banpling Procedure

Sampling the solid traps, except the plutonium trap, was done by
passing the solids through a fumnmel with an inverted "Y" bobttom until
a sample of convenient size (about 7 o exceplt in the case of the
fluidized-bed sample, which was 3.5 ¢} was obtained. Two samples from
ecach trap were submitted for analysis, and the results were averaged.
The funnels used for this procedure were washed prior to the sampling
step; and, In each run, the "coldest" traps were sampled first as a
Turther precaution against cross-contamination. Such sampling was
unnecessary Tor the plutonium trap since each section of the Trap

contained only about 2.5 g

The filter of the fluidized-bed reactor was leached after each
run with 100 ml of 2 N A1(1\103)3
was submitted for analysis. The,UFé oroduct in the cold trap was
hydrolyzed with 200 to 250 ml of 1 I Al(1\103)3.

ctarted at eilther 30°C or —80°C, and then the temperature was increased

solution, and a sample of the leachate
This hydrolysis was

Lo 100°C for about 30 min. A more complete recovery of the uranium
in the solution was achieved when hydrolysis was begun at 30°C. A
sample of the resulting solution and s sample of a water rinse of the

cold btrap was submitited for analysis.

Samples of the scrub solutions were also submitted for analysis.
10

2.3 Experimental Materials

A1l metal vessels, excepht the scrubber, were fabricaled of nickel;

the scrubber was constructed of Alundum and stainless steel.

The heat-transfer medium in the fluidized-bed reactor consisted

of 50 g of 48- to 100-mesh Alcoa T-61 alumina.

The fuel charge, which consisted of about 34 g of UOE from the
Yankee rvezctor, had been irradiated to a burnup of about 34,000 Mwd/
metric ton and cooled for two years. The estimated composition of
this fuel, as calculated by Merriman's program,l is given in Table 1.
In general, these values were used in the calculations presented in
this report. The isoltopic analysis of the plutcnlum in this fuel, as

determined by mass spectrographic methods, is given in Table 2.

The Naf used in the traps (except the plutonium trap) consisted
of 1/8ainu right circular cylinders obtained from the Harshaw Chemical
Company. In the plutonium trap, brcken pellets or fused NaF, 12 to 20

mesh in each case, were used.

Part of the MgF2 used in the technetlium-neptunium trap was
obtained from the Paducah Gasecous Diffusion Plant; the remainder was

prepared at ORNL by fluorination of MgSQu.
3. RESULTS AND DISCUSSION

3.1 Oxidation of Fuel

Before the start of Tthe oxidstion, the Tuel was Tirst heated to
450°C in fluidizicg nitrogen. The oxidation treatment with 20 vol % 02
in nitrogen lasted for 2 hr at 450°C and resulted in pulverization of
the fuel (see Fig. 5). During the heatup period and the oxidation, about
95% of the tritium was evolvedng The Initizl tritium content was deter-
mined by dissolving a 6-g bateh of fuel in nitric acid and analyzing
the solution and off-gas for tritium;g the amount of tritium remaining
after oxidation was determined similarly. No significant amounts of
other materials, excepi the rare gases (which were not determined),

egcaped from the fluidized-bed reactor.
i ' 2 A - » " . 9 9)
Table 1. Estimated Composzsition of 3hug Charge ™ of Yankee UO2 Fuel

 

 

Element me dis/min
U 28, 600
b
Pu 374
Np 2.5
Rb 10.4 ~ 0
]

Sr 25.0 §.72 x 107F

- - 10
71 106.5 2.25 x 10

-
Nb 6.29 x 107 5.01 x 10°°
Mo 103.5 ~ 0
O

Te P64 107
Ru 65.2 8.0l x 1077
Te 17.7 3.h3 % 10t
Cs 11k.3 7.65 x 1072
Ce 73.8 1.03 x 1013
3g” 1.15 x 100t

 

a . . X
"'uel had been irradiated to a burnup of
34,000 Mwd/metric ton and cooled for two years.
b . - ,
From unpublished data of J. H. Goode,
ORNL.
12

Table 2. lsotopic Analysis of Plutonium™ in Yankee UOE Fuel

 

 

Isotope At. %
238 2. 36
239 57.75
2Lo 20.60
241 13.78
2o 5.52
2l < 0.001

 

adis(a)/(min (mg Pu) =

! )
1000 % 107 {caleulated).

3.2 Volatilization of Uranium with BrF

The uranium volatilization step is shown in TFig. 6. In this
step, which was carried out at 300°C, the treatment typically consisted
of exposure to 5 vol % BrF5 for 1 hr, 10% BrF5 for 2 hr, and 5% BrF3
for 0.5 hr; in ecach case, the BTF5 or Br’F3 was diluted with nitrogen.
After the gas contalning the volatile fission product fluorides, UF6,
bromine, and bromine fluorides leaves the fluidized~bed reactor, it
enters the bottom of the CRP (complexable reaction products) trap,
vhere 1t is mixed with excess fluorine to convert the bromine to BrF5.
This prevents loss of uranium in the CRP trap via formztion of non-
velatile UF5 complexes. In our experiments, an average of about 0.02%
of" the uranium was found in the CRP trap. Most of the volatile fission
product Tluorides are removed in this trap. The gas then passes through
thie uranium sorption traps where uranium, techretium, and some molybdenum

are sorbed. Finally, the gas is routed to the scrubber, where the

Tluorine =znd bromine flucrides are contachbed with KOH-KI solution.

Treatment with BTF,3 for a briefl pericd at the end of the uranium

voelatilization step has been found to be desirable for the cleanup of
13

 

ORNL DWG, 6¢9-92

 

 

 

 

 

BLOWBACK TO OFF-GAS
SCRUBBER
100°C
| 450°%C
2 hr 20%
02 IN No

 

F'ig. 5. Oxidation Flowsheet.
BLOWEBACK

1 hr 5% BI’F5

2 hr 10% Brfg
0.5 hr 5% BrF3

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

ORNL DWG €9-1268

 

 

 

 

L TO OFF-GAS
l I SCRUBBER
CRP U u
100°C Trap |400% | |Sorptiont |25 | [Sorption| |25°C
KBockup)

Ti T2 T3
N Ny 300°C
IN N2
IN N2 Fp L ]

250-g NaF 250-9g NaF 250-g NaF
Residence Time: 2.5 Sec 4 Ssac 4 Sec

Fig. 6. Uranium Volatilization Flowsheet.
o

uranium. In Fig. 7 the amount of uranium found in the fluorination

; treatment) is plotted vs the BTF3 treat-

ment time. When no BrF, treatment was used after the BrF_. volatilization,
J

step (subseguent to BrF5~BrF

ahout 3% (~ 960 mg) of the uranium charge was left in the fluildized-bed
reactor. However, when a 0.5-hr trestment with 5% BrF3 in Né vas used,
about 80% of this residual uranium was removed. The utility of BrF3

lies in its ablility te [luorinate uranium at a lower temperature3 than

BrF5,

lines. Bromine trifliuoride also leaves less uranium on the alumina.

thereby allowing cleanup of the disengaging system, Tilter, and
3
The very high point at 3 hr exposure is probably due to an experimental

error oy some analytical errcr.

oince ruthenivm fluoride was the major, high-activity, volatile
fission product fluoride present in our exzperiments, 1t was studied more
extensively than the other fission product flucrides. Figure 8 is a
semilogarithmic plot showing the amount of ruthenium that was volatilized
during the fluorine treatment ve the equivalent number of liters of

BrF. passed through the bed during the uranium volatillzation step.
2

(Here, one volume of BrF., is considered to be equal to 0.6 volume of

3

rFS.) This plot should be linear if the volatilization of ruthenium

5

o

-

2 Tirst-order reaction with respect Lo the amount of ruthenium
remaining in the fluidized bed. This is seen to he approximately true.
The importance of these data lles in the Information they provide con-
cerning the handling of a plutonium stream containing ruthenium. It
would be advantsgeous for the ruthenium to be volatilized with the
vranium. In our experiments, about 90% of the ruthenium was volatilized
with 6.7 liters of BIFS; this required 33 min of treatment with 10 vol %
rF_ in nitrogen. For every additional 32-min periocd of BrF

>

the ruthenium DF was increased by a factor of 10.

treatment,

2

Ruthenium-106 was the only sgignificant gamme emitter found in the
CRP trap when the trap was counted with a lead-shielded Geiger tube.
Figure 9 shows a plot of the fraction of the gamma activity vs the equiv-

alent Tluorine volume. In this plot one volume of BrF5 ig assumed Lo
o and one volume of BrF3 1s considered

e equal to 2.9 volumes of F
1.5 volunmes of Fp“ When an all-fluorine {lowsheelt was

equivalent to
16

ORNL DWG. 69-556

 

 

 

 

 

 

 

 

 

 

 

1000 |
&
2
A 800
=
Q L
& ;
Iij 600 J—
z L
o |
Z 1;
Z |
< 400 S —
2 ;
&
D -
o
£ @
200k \\ ,,,,,,,
\9
0 | |
O 1 ’ 3
TIME OF EXPOSURE TO 5 vo! 9% BE., (hr)

3

Fig. 7. Residual Uranium vs BrF3 Exposure.
17

ORNL DWG. 69-558

 

T~ INITIALLY IN FUEL CHARGE

 

-
N

 

O

N\

[ TTH

!

i

/

 

O

Pl

|

S

 

o

1;O()Ru VOLATILIZED IN PLUTONIUM VOLATILIZATION STEP (dis/min)

|

1

l

|

 

 

 

 

 

 

0 2 4 6 8 10 A2 14 16 18 20
EQUIVALENT LITERS OF BrF5

 

Fig. 8. lO6Ru Found in Pu Volatilization ve Exposure to BrF_ in

Uranium Volatilization Step. ‘ . 2
]
QUANTITY OF OéRu IN CRP TRAP (°5)

qee

w
o

N
O

o
Q

20

ORNL DWG. 69-557

 

 

 

 

 

 

o0

 

 

o_p
O
5 O ] BrF, AND BrF ,
O /
O O O
O —
O

 

 

 

 

 

® VOLATILZED WITH F2

VOLATILIZED WITH BeF

 

 

 

 

| & ’ O 5 OR &FS
| |
. | _ .
|
|
e o]
8 10 iz 14 16 i8 20 22 24 26 28 30 32 34 36 38
EQUIVALENT NUMBER OF LITERS OF F2
Fig. 9. Rate of Appearance of iO6Ru in CRP Trap After Volatilization

with Br¥, BrT

37 or Fg.

qL
19

tested, the ruthenium activity reached ite maximum very rapidly (see
Fig. 9). With Br'B, an initial rapid increase wag Tollowed by a slow
linear increase. A likely explanation for the elow linear increase
is the transpiration of a compound having a relatively low volatility.
Assuming that this compound is RUFS, The results indicate that the
temperature of transpiration is asbout 55°C using the re_‘;_:)orted)Jr vapor
pressure of RuF5 and knowing the weight of ruthenium being picked up
by the trap. This temperature corresponds to that of the line between
the fluidized-bed reactor snd the CHP trap, and indicates that the RUF5
ig deposited there. These indicatlons were confirmed by serious radisz-
tion damage to this line and by radiochemical analysis, which showed
that, at the end of the volatilization step, about 20% of the total
ruthenium could be Tound on the inside of the line. Visual observation
showed that the line used during. the all-fluorine test was only slightly
discolored, indicating that only a small guanbtity cof ruthenium was
deposited in it. Therefore, 1t seems likely that treatment with BrF5
produces a greater quantity of low-volatlility ruthenium compounds thsn
Tluorine treatment does.

Fission product DF's for the CRP trap sre listed in Table 3. In
the Firet "hot" vun (run 3) the DF'e {except for cesium) were each
about 2000, Theze values are quite high, considering that the residence

time for the gas in contact with the 400°C WaF was only sbout 2.5 sec,

Table 3. Fissgion Product Decontamination
Factors Tor the CRP Trap

 

Decontamination Factors

 

 

Ty A
Run No. Gross 7 Gross B LOORu Cs
3 1790 2610 2000 2.0
L 6.1 5.8 6.4 ~ 4.0
5 13 Il 30 1.8
6 15 33 92 3.1

 
20

Tn later runs, desplte the sampling precautions mentloned earlier, the
DF's decreaged significantly. The most likely explanation for the
lower values is cross~-contamination since all of the higher DF's
decreased to about the same level. We believe that the IDF's from the
first hot run (No. 3) are "true" values (i.e., they are the values that

could be cxpected in the absence of cross-contamination).

One undesirable result of the BTF5 treatment was the small amount
of plutonium found in the CRP trap in each run. Table i compares the
percentage of the total plutonium found on this trap with the percentage
of the total 908r found there. It was felt that these quantitlies should
be about equal since neither plutonium nor 9OSr is expected to be

volatilized by BrF
90

5° Surprisingly, the loss of plutonium is about ten
times that of “ Sr; one possible explanation for this is that the Pth
particles are considerably smaller than the Sng particles and are,
consequently, preferentially blown thvough the filter. The presence

of plutonium in the CRP trap was confirmed by differential pulse-height

analysis.

Table 4. Plutonium Entrainment, as Compared with
Sr Entrainment, by BTFS—Né Stream

 

 

9OSr Transferred P Transferred Pu/gOSr
Run HNo. to CRP TT%S to CRP Trap Percentage
(% of total “MSr) (% of total Pu) Ratio
-0 '
3 2.h x 10 0.4 17
L 1.4 x 1077 C.1 T
-
5 1.6 x 10 ~ C.1h 9
6 3.0 x 1077 0.25 8

 
3.3 Desorption of Uranium

Desorpticon of the uvranium was asccomplished by connecting the main
wranivs sorption trap {(T2) to a 400°C NaF polishing trap {Th), a 100°C
MgFP trap (TS), and a cold trap ccoled to —80°C. This arrangement is
shown in PPig. 10. Fluorine was passed through the traps st the rate
of about 100 ml/min. Reliable values for the fission product DF's for
the sorption-descrption are not availasble becauze of the small quantities
of fission products present and because of the cross-~contamination prob-
lem mentioned previously. However, overall Tission product DF's for the
uranium product were gbtainedj and are listed in Table 5. It appears
that DF's of avout 107 are caslly obtained for many contaminants with
this process. Molybdenum was partially removed by virtue of its tendency
not to cosorb with uranium during the BrF5 volabtilization step. The
plutonium DFfs are encouraging since they indicate that the uranium

product could be treated as plutonium-free material during subsequent

handling.

—

The technetium DF'g for trap 5 are given in Table 6. Four-mesh
MgFP from the Paducah Gaseous Diffusion Plant was used in the traps
for runs 3 and 4. In run 5, we used 12~ Lo 20-mesh materizsl that had
been prepared at ORNL by fluorinsting MgSOA. The smaller particles
gave much better results, probably because of thelr greater external

surface area. Contact time was sbout 15 sec.

The overall uranium maberial balances (see Table 7) were not
satigTactory in all cases. Data in the table suggest that the
difficulty may be caused by starting the hydrolysis at a low temperature.
The explanation for the uaiformly low material balances, except in the

case of run 5, is not known.

3.4 Volatilization of Pqu with Fluorine
-

In the plutonium volatilization step, the fluidized bed was
treated with elemental fluovine, as shown in Fig. 131, to form veolatile
PuFy.  Tn the cold tests and in the first two hot tests (runs 3 and &),

fluorination was started at 300°C, After sintering and actual igrnition
 

 

 

 

ORNL DWG 68-93

 

 

 

 

 

 

 

 

 

125°
TO .
430°C Te
4 hry
100 mi/min Fop

 

 

Residence Time:

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

U
POLISHING Tc-Np COoLD
TRAP TRAP TRAP TO OFF-GAS
SCRUBBER
{
I
5
T4 T5 |
i
|
i
50g NoF  30¢g MgFo -80°C
400°C 100°C
5.5 Sec 15 Sec 4 Min
Fig. 10. Uranium Desorption Flowsheet.

co
Overall

Decontamination Factors for the Uraniwn Product

 

Decontamination Fachors

 

 

Run Gross Gross 196 %G Total
» A ./'. 1T A
No. ¥ B Ru Cs Sr Rare Earths Te Mo Pu
} s
-t 4 - flflo
x 10 x-;@5 % 10
6 g 5 6
-~ ~ — . < —~ -, = —~. - — i,
3 1.3 x 16 L.9 L.g 2.6 x 10 2.8 x 10 2 x 10 .6 8.3 I
‘ | 5 5 5 . k . .~
L 1.2 x 10 3.3 2 1.4 x 10 10 8 x 10 G.5 2.5 3 D
7 3.5 x 10 1.35 x 107 i

N

7.3

 
Table 6. Decontamination Factors for Technetium,
Using a 100°C MgFE Trap (Trap 5)

 

 

Te Mesh Size of
Run No. DF MgF2
3 1.09 ah
Iy 1.31 12 to 20
5 2.15 12 to 20

 

Table 7. Uranium Materisl Balances

 

 

 

Cold Initial
Run U Trap Total for Hydrolysis
No. Charged Amount U found No. Cold Trap Temp.
(g) (g) (%) (%) (°c)
1 2G.6 06.6 0 1 20 30
3 7.2 20 .4 75 2 —80
I 2G,7 217 73 2 95.7 —80
5 28.0 39.2 140 2 30
6 26.7 oo & 93.2 + 7.5 None No desorption

26,9 21.7 + 0.6 80.7 + 2.0 None Nc desorption

 
 

BLOWBACK

 

 

 

 

 

 

 

 

 

 

 

 

 

 

TO OFF-GAS
SCRUBBER
300°C
325°C
-4 OR
550°C
o TWO 2.5"0
380 NaF BEDS
F2 IN N2 5 hr - _
Residence Time: 0.02 Sec Each

 

Fig. 11. lutonium Volatilization Flowsheet.

ORNL DWG 69-1267

¢z
26

of the alumina occurred in runs 3 and L4, respectively, conditions for
this step were modified. In the later tests, fluorination was begun

at about 200°C, with the fluorine concentration (in nitrogen) programmed
from 10 to 50 vol %. Ihe temperature was then increased to 300°C over
about a 30-min period; 50 vol % F, was used. DNext, the fluorine concen-
tration was incressed to 100% over a subsequent 30-min period. Finally,
the temperature was raised to 500°C over a 1-hr period and maintained

at 500°C for 2 hr. The total fluorination program required 5 hr, of
which 3.9 hr was at a temperature of 300°C or greater. When this program

was followed, no sintering of the alumina was observed.

Plutonium is readily removed from the {luorine stream by a very
small NaF trap. In our experiments, g 2.5-g NaF trap at 550°C sorbed
about 99.9% of the plutonium that reached it. The residence time for

the gas was only about 0.02 sec.

The major fission product that cosorbed with the plutonium was
rutheniuws; after ruthenium, cesium was most Important. The overall
ruthenium and cesium DF's are shown in Table 8. The cesium DF is
relatively high (about lOu), and ceslium could be easily separated from
the plutonium during its removal from the NaF (possibly by dissoluticn
of the NaF in anhydrous HF). Thus ruthenium is likely to be the most
troublesome. As was mentioned earlier in connection with the inter-

halogen flowsheet, the amount of ruthenium that is cosorbed with the

Table 8. Overall Ruthenium and Cesium Decontamination
Factors for Plutonium Product

 

 

 

Run Temp. of Ru Ratio of DF Cs
No. DPu Trap 106Ru DF to DF in 13M,137CS DF
(°¢) (dom/mg Pu) Run 3 (dpm/mg Pu)
3 325 2.67 x 108 76 6.7 % 10/ 273
325 1.21 x 107 17 0.22% < 2.7 x 10 5 6.8 % 103
~ =
6  ~ 550 3.85 x 100 5250 697 1.8 x 100 1ot

 

a . , . . -
Ratios expected from the amount of ruthenium found and the differ-
cnce jn trap temperature: 0.306 (run 4) and 45 (run 6). (By Re’. 5)
plutonium can be easily reduced by extensive treatment of the Tluldized
ved with BrFS. Another method Tor reducing the amount of cosorbed
ruthenium would be to cperate the plutonium sorption bed at a temperature
that is unfavorable for ruthenium sorption: Tor example, it is known

that ruthenium sorption on Na¥ decreasges significantly at temperatures

5

above 500°C, However, in an experiment in which the NaF was heated
to about 615°C, severe sintering was cbserved; this was probably the
result of the Tormation of the N’aF—-PuFlL eutectic. Thus, 550°C seems
to be about the highest usable temperature. At 550°C, the ruthenium
DF (6.0) achieved in the plutonium trap was four times that obtained
at 325°C (1.5). Thus, for plutonium decontamination the best recom-
mendation is to fluorinate for a fairly long period of time with

Brf_ and to operate the plutonium trap at about 550°C.

5

Plutonium material balances were not uniformly good (see Table 9).
Tn run 1, which was a "cold" run, the exact plutonium content (262 mg)
was known. A 93% material balance iz considered acceptable for this
gquantity of plutonium. However,'material balances for runs 3 and 4 are
poor. No material balance is available for run 5 because the plutonium

trap was lost. DMaterial balances for runs 6 and 7 are quite satisfactory.

Table 9. FPlutonium Materizl Balance

 

 

 

 

Pu Found in
Run Fluidized-Bed Reactor Total Pu Found
No. Pu Charged me, % of Pu Mg % of Pu
(mg) Charged Charged
1 o2 6.6 2.5 o, 1 93.2
3 355 70O L 18.9 202 79.4
L 388 22.9 5.6 302 7.6
6 349 104 28. 4 396.7 113.7
7 352 208 + b 56,3 + 11 333.3  9k.5 + 11

 

a . . . . -

Based on analyses of plutonium in fuel (11 mg of Pu per g
of fuel) by J. Goode, except in run No. 1 where plutonium was
weighed outb.
All-Fluorine Flowsheet

 

An alternative to the interhalogen flowsheel 1s the alli-fluorine
Tlowsheet 1in which both the uranium and pilutonium are volatilized, as
UF6 and ]?11}-“6q by using fluorine. 1In one possivle version of this Tlow-
sheet the plutonium is removed from the [luorine stream by a small high-
temperature NaF trap located immediztely behind the fluidized~bed
reactor. The remaining gas passes through the traps for the uranium

volatilization step, as discussed previously.

In the hot-cell test of this Tlowsheet, the plutonlum trap was
operated al zbout 620°C. Unfortunately, before the run was completed,
this trap plugged, apparently due to the formation of a molten NaF—PuFM
eutectic salt. At this point only about 35% of the plutonium had been
volatilized; about two-thirds of the 10 Ru and almost 211 the uranium
had been volatilized when the run was terminated. Based on this partial

run, we can make the following statements:

(1) A more effective decontamination of plutonium from ruthenium
was achieved than was eXpected..

(2) An overall ruthenium DF of 249 was obtained; about 200 of
this wvalue is attributable to nonscorption of ruthenium in
the plutonium trap.

(3) Routine operation of the trap at 620°C would probably be
difficult because of the plugging and sintering that would

ke encountered.

A previous run using the interhalogen flowsheet with a plutonium trap
at about 550°C gave a lO6Ru DF of only about 4.0; whether the higher

DF in the all-fluorine case is the result of the presence of a larger
amount of ruthenium (2bout 60 mg as compared with about 0.6 mg) or to

the higher temperature 1s not known.
29

3.5 Recovery of Plutonium from NaF Trap

After the PuF6 igs collected on NaF, the plutonium must be recovered
from the complex that is formed. One possible method consists of aqueous
dissolution followed by ilon exchange treatment. Another method involves
dissolution of the NaF with anhydrous HF, leaving Pth as an insoluble
residue; this treatment also gives a significant additional ruthenium
DF. The second method was tested with the plutonium trap from run 6. 6
As a pretreatment the NaF was first fused in a platinium crucible at
about 1050°C. A ruthenium DF of sbout 2 was obtained as & result of
ruthenium plating on the crucible. [Use of a more-reactive crucible
(e.g., nickel) would probably have given a higher DF.] When the NaF
was dissolved in anhydrous HF, an additional ruthenium DF of 2.6 was

cbhtained.
. :CONCLUSIONB

Based on the hot-cell work, the fluidized-bed volatility process
appears to be chemically feasible. Care must be exercised at the
start of the fluvorination step to prevent sintering of the alumina
bed. ILarger equipment would probably present an even grealer problem
in this respect since the heat transfer would be less effective.
Ruthenium contamination of the uranium product should be low since
ruthenium DF's of about 106 were found in the hot-cell experiments.
Ruthenium contamination of the plutonium product can be reduced by
removing most of the ruthenium with the uranium during the BrF5
treatment. A more effective separation of plutonium and ruthenium
is achieved by operating the plutonium trap at about 550 to 580°C
(instead of at 325°C).
1.

30

5. REFERENCES

A, A, Chilenskas, Argonne Natlonal Laboratory, personal

communication.

J. H. Goode, CRNL, unpublished dats.

D. 0. Rester, Coc-op Student at ORNL from Mississippi State

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H. A. Bernhardt, et al., The Preparation of Ruthenium Pentafluoride

 

and the Determination of Its Melting Point and Vapor Pressure,

ARCD-239C (Nov. 1948).

 

E. D. Nogueira and G. I. Cathers, Sorption of Fission Product

 

(Niobium, Ruthenium) Fluorides on Sodium Fluoride, ORNI-TM-2169

 

in press).

Test performed by M. R. Bennett, ORNL.
*

H
TN o= OV o D e

F b e
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19.
20 .
27,
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23-
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6.
7.
8.
9.
30.
31.
32.
33.

35-
36.
37-

39.
Lo,
L.
Lo,
12
hh,
h5.

¢1F1C2€3fi$iifil§ E:F’?ifiiliiiw =M HgHS oSSR oEagSYT 0 QK

*

&

.

Adams
. Adamson
Arnold
. Bennett
. Berry
Blanco
Blomeke
. Bomar
. Bond
. Boyd
. Bradley
Brooksbharnk
Brown
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Burch
Carr
Cathers
Carter
Chandler
Clinton
Coleman
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Culler, Jr.
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vig, Jr.
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Hzas
Balre
Hammond
Harms
Haws
Horner
. Hurst

>

a

gihlgiflifl’fi!3121fi HESWEE»>> OO HW XY E =

HE

»

UEOQOHOQ PO THREE SN QF

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DISTRIBUTION

Internal

GRS Y G "G g Y s Y tu$>C>?2EI&%E+&1E1$=EifiifijfiiLihii’b‘H;z QX O g

O e

PO YOO oS yOogORr A nNnERESTD T

SO =200

Trvine

. Kappelmann
. Kasten

Kibbey
Kitts

. Lamb

Leitnaker
Leuze
Lisser
Lioyd
Long

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McBride
McClung
McCorkle

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Milford
Moore
Morse
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Nicholson
Notz

Odom

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Pattison
Pechin
Prados
Pratt
Rainey

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Ryon

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Scobt
Sease
Shappert
Siman-Tov
Snider
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138.
139.
140,
141
1he.
143,

144,
1hs,
1h6.

1h7.
148,

149,
150.
151.

152.

153.
154,
155,
156,

157.
158.
159.
160 .

32

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94, W. C. T. Stoddart 107. W. M. Woods
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Iibrarian, AAEC, Res. Estb., Private Mail Bag, Sutherland, N.S.W.,
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R. H. Burns, X. D. B. Johason, W. H. Hardwick

A. Amorosi, ANL, IMFBR Program Office

R. H. Ball, RDT-0OSR, P. 0. Box 2325, San Diego, California 92112

R. G. Barnes, General Electric Company, 283 Brokaw Road, Santa Clara,
California 95050

C. B. Bartlett, AEC, Washington

Franc Baumgartner, Professor fur Radiochemie, Universital Heidelburg,
Kernforschungszentrum, Karlsruhe, 15 Karlsruhe, Postfagh 9&7, West
Germany

W. G. Belter, AEC, Washington

D. E. Bloomfield, Pacific Northwest Laboratory, Richland, Washington
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Leslie Burris, Jr., ANL

M. Benedilct, Massachusetis Institute of Technology

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Seine, 90, France

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161,

162.
163.
1604,
165.

166.

167.
168.

169.
170.

171.
172.
173,
17k,

175.

176.
7T,
178.
179,
180.

181.

182.

183,
184,
185.
186.
187.
188.
189.
190.

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192.

193.
194,

195.

33

C. R. Cooley, Pacific Northwest Laboratory, P. 0. Box 999,
Richland, Washington

'D. F. Cope, RDT Site Office {ORNWL)

E. A. Coppinger, Paciflc Northwest Laboratory, RlchldHQ, Washlngton
J. Crawford, AEC, Washington

G. W. Cunnlngham, AEC, Waeshington

C. B. Deering, AEC- ORO

Paul Dejonghe, CEN, Boeretang, 200, Mol, Belgium

W. Devine, Jr., Production Rea¢tor DlVlSlOH, P. 0. Box 550,

‘Richland, Wauhlngton Q9352

E. W. Dewell Babcock & Wilcox, Lynchburg, Virginia
Stanley Donelson, Gulf General Atomic, P. 0. Box 608, San Diego,
California ‘ '
Furastom, Casella Postale No. 1, Ispra, ITtalia; Attn: M. Lindner
Burochemic, Mol, Belgium; Attn: FEurochemic Library

Yehuds Feige, Minister of Defense, AEC, Rehovoth, Israel

Pnilip Fineman, Argonne Natlonal Taboratory, East Area EBR-2,
National Reactor Testing Station, Scoville, Idaho
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J. C. Frye, State Geologlcal Survey Division, Urbana, Illinois

W. P. Gammill, AEC, Washington
Ray Garde, Los Alamos |
R. M. Girdlexr, E. TI. du Pont, SRL

Simcha Golan, Atomics International, Canoga Park, California

J. J. Goldin, Mound Iaboratory, Bldg. A, Room 159, Miamisburg,

Ohio 45342

A, J. Goldjohn, Gulf General Atomic, P. 0. Box 608, San Diego,
California '
R. H. Graham, Gulf General Atomic, San Dlego, California

J. S. Griffo, AEC, Washington

H. J. Groh, E. I. du Pont, Savannah River Laboratory

Norton Haberman, RDT, AEC, Washington

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P. 5. Holstead, RDT-OSR, P. O. Box 550, Richland, Washington
C. H. Ice, E. I du Pont, SRL

Michio Ichikawa, Tokai Reflnery, Atomlc Fuel Corp., Tokal-MUra
Ibaraki-Ken, Japsn

C. J. Jouznnaud, Fuel Reprocessing Plant, CEN, B.P. No. 106
30~ Bagrwlg/cage, Marcoule, France

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Idaho Falls, Idaho 83401

A. 5. Kertes, The Hebrew University, Jerusalem, Israel

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Godesberg, West Germany

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Fuels Section, Chemical Technology Division, Juelich Nuclear
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Leopold Kuchler, Farbwerke Hoechst AG, Frankfurt (M) Hoechst,
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200 ,
201,

202.
203.
20U,
205,
206.

207,
208.
209.
210.

211.

212,
213.
21k,

215,
216.
217.

218.

219.
220,

221.

222,
223.
20k,
225,
206,
227 .

228.
229,

230.
231.

232.
233.

o3,
235,

34

S. Lawroski, Argonne National ILaboratory

R. E. Lerth, Pacific Northwest Laboratory

W. H. Lewis, Vice President, Nuclear Fuel Services, Inc., Wheaton,
Maryland 20902

T. McIntosh, AEC, Washington

H. A. C. McKay, UKAEA, Harwell, Berks, United Kingdom

W. H McVey, AEC, Washington

S. Marshall, National Lead Company of Ohio

A. R. Matheson, Gulf General Atomic, P. 0. Box 608, San Diego,
California

Ken Mattern, AEC, Washington

. Lopez-Mechero, Eurochemic, Research Dept., Mol, Belgium

R. L. Morgan, AEC-SROO

R. T. Newman, Allied Chemical Corp., General Chemical Div.,

P. 0. Box 405, Morristown, New Jersey 07960

Eduardo D. Nogueilra, Seccion de Combustibles Irradilados, Junta
de Energia Nuclear, Ciudad Universitaria, Madrid-3, Spain

R. E. Norman, CRNL (GGA employee)

Laboratory and University Division, ORO

D. A, Orth, E. I. du Pont, Savannah River Plant, Aiken, South
Carclina

R. E. Pahler, AEC, Washington

F. L. Parker, Vanderbilt University, Nashville, Tennessee

N. Parkinscn, Experimental Reactor Establishment, UKAEA, Dounreay,
Scotland

Baldomero Lopez Perez, Doctor en Quimica Ind., Centro de Energia
Nucl., Juan Vigon, Ciudad University, Madrid-3, Spain

R. L. Philipporne, RDT, ORNL Site Rep., AEC

A. M. Platt, Pacific Northwest ILaboratory, P. 0. Box 999,
Richland, Washington

W. H. Reas, General Electric Co., Vallecitos Ilaboratory, Pleasanton,
California

W. H. Regan, AEC, Washington

P. J. Regnaut, CEN, Fontenay-aux-Roses, Paris, France

R. F. Reitemeier, AEC, Washington

C. W. Richards, AEC, Cancga Park, California

I. C. Roberts, AEC, Washington

Theodore Rockwell ITII, Chariman, AIF Safety Task Force, MPR
Associates, Inc., 815 Connecticut Avenue, N.W., Washington, D. C. 20006
0. T. Roth, AEC, Washington

Bruce L. Schmalz, Atomic Energy Commission, P. . Box 2108,

Tdaho Falls, Idaho 83401

A. Schneider, Allied Chemical Corp., Industrial Chemicals Div.,
P. 0. Box 405, Morristown, New Jersey 07960

W. F. Schueller, Technicel Maznager, BMWF Scientific Research,
7501 Lecpaldschafen, Karlsruhe, Germany

Harry 5. Schneider, AEC, Washington

Giancarlo Scibona, Centro di Studi Nucleari della Casaccia, Rome,
Ttaly

Jitender D. Sehgel, Bombay, India

M. Selman, Nuclear Malerials and Eguipment Corp., Apollo, Pennsylvanis
15613
236.
237.
£38.

239,
210,
ol

oho,
b3,

250,
D51,

252,
253,
o5k,
055,

256,

257.
258,

259.

260 .
261.
P62,
63,
o6k,

265,
066,
D67 .
2608.
269.
570,

271.

272.

35
;
i

J. J. Shefeik, General Dynamics, San Diego, California

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Atou Shimozato, Nucl., Reac. Des. Sect., Nucl. Power Plant Dept.,
Hitachi ILtd., Hitachi Works, Hitachi-Bhi Ibaraki-Xen, Japan

C. S§. Shoup, AEC, (RO

E. E. Sinclair, AEC, Washingbon

W. L. Slagle, Water Reactor Safety Program OfTice, Phillips
Petroleun Co., Idaho Falls, Idaho 83401

C. M. Slansky, Tdaho Nuclear Corp., Idaho Falls, Idaho

Pedericc de ILora Soria, Grupo de Combustibles Irradiados, Junta

de Energia Nucl., Div. de Mat., Ciudad University, Madrid-3, Spain
Narayanan Srivivasan, Head, Fuel Reprocessing Division, Bhabha
Atomic Research Center, Boubay, India

F. Stelling, Gulf General Atomic, P. 0. Box €08, San Diego,
California 92112

C. E. Stevenson, Argonne Natlonal Laboratory

K. B. Steyer, Gull Genersl Atomic, P. O. Box 608, San Diego,
California 92112

¢. L. Storrs, Abomics International, Division of North American
Aviation, Inc., P. Q. Box 309, Canoge Park, California 91305

J. A. Swartout, Union Carbide Corporation, New York, New York
Jacob Tadmore, Israel Atomic Energy Commission, Sored Nuclear
Research Center, Yavne, Israel

X. L. Talmont, Plant of Irradiated Fuels Treatment, Centre de la
Hague, Cherbourg, France

V. R. Thayer, E. I. du Pont, Wilmington, Delaware

K. T. Thomas, Atomic Energy Establishment, Trombay (Bombay), India
R. E. Temlinson, Atlantic Richfield Co., Richland, Washington

L. B. Torobin, Standard 01l Company of New Jersey, 30 Rockefeller
Plaza, Room 1711C, New York, New York 10020

C. A, Trilling, Atomics International, Div. of Nerth American
Aviation, Ine., P. 0. Box 309, Canoga Park, California 91305

E. J. Tuthill, ANL

Director, Division of Naval Reactors, U. S. Atomic Energy Commission,
Washington, D. C. 20545 Attn: R. S. Brodsky

R. P. Varnes, Combustion Engineering, Inc., Nuclear Divisilon, P. Q.
Box 500, Windsor, Connecticut 06095

R. C. Vogel, Argonne National Laboratory

W. R. Voight, AEC, Washington

E. BE. Voiland, Pacific Northwest Leboratory, Richland, Washington
R. D. Walton, Jr., AEC, Washington

B. ¥. Warner, UKAEA, Technical Dept., Windscale, Sellafield, Cumb.,
United Kingdom

M. J. Whitman, ALC, Washington

W. E. Winsche, Brookhaven Naticnal Laboratory

H. 0. G. Witte, KFA-heisse zellen, Juellich, Germany

J. N. Wolfe, AEC, Washington

John Woolston, AECL, Chalk River, Canada

D. L. Ziegler, Dow Chemical Co., Rocky Flats Division, P. 0. Box 888,
Golden, Colorado 80401

M. Zifferero, Comitato Nazionale per L'Energle Nucleare, Via
Belisaro, Rome, Ttaly

L. H. Meyer, E. I. du Poent, SBRL