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ORNL-TM-3464.txt
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”.-'--.’_'.7:-0A|< RI_DGEV 'NATIONAL I.ABORATORY
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| f__;_umon CARBIDE conponmon . NUCLEAR nwssnon}_ Gy
u s ATOMIC ENERGY commassmN
ORNI. TM 3464
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. XENON BEHAVIOR IN THE MOLTEN SALT REACTOR EXPERIMENT
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P i TR " ™ e " ik " Ty
s i [ e [ . Vo e - . T VoL i L . i S . C S . B s - oo nf D 5 :
'-NDIIBET"IIS document eontams mformahun of a prelammary nuture S
" “and was prepared primarily for internal use at the Oak Ridge Nahonol -
Luboro'rory At s sub[ect io revasuon or correchon und iherefore does L
not represent a fmoE rep : — : o
RGT S
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 Commission, nor any of their employees, nor any of their contractors,
‘subcontractors, or their employees, makes any warranty, express or imblied, or |
assumes any legal liability or responsibility .for the accuracy, completeness or
usefulness of any information, apparatus, product or process disclosed, or
represents that its use would not infringe. privately owned rights.
v)
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ORNL-TM-3464
Contract No. W-7405-eng-26
REACTOR DIVISION
J. R. Engel
= —-———-—-—"" NOTIC E...__..—-—-—————- :
‘| This report-was ‘prepared as an ‘account of work
‘ sponsored by the United States Government. Neither |.
. | the United States nof the United States Atomic Energy
. | Commission, nor -any-of thei,r.e,mployees, nor any of .| -
‘1 their contractors, subcontractors, or their employees, | -
‘1 makes any warranty, express or implied, or assumes any
- | ‘egal- liability or. responsibility for the .accuracy, com-
| pleteness or usefulness of any information, apparatus,
7 -product or process ‘disclosed, or represents that its use
1 ‘would not infringe privately owned rights. ’ v
XENON BEHAVIOR IN THE MOLTEN SALT REACTOR EXPERIMENT
R. C. Steffy
L el
OCTOBER 1571
OAK RIDGE NATIONAL LABORATORY
- 0ak Ridge, Tennessee
~ operated by
UNION CARBIDE CORPORATION
- FOR THE
* U,S. ATOMIC ENERGY COMMISSION -
7
GISTRIBUTION OF THIS DOUMENT 15 URL
TTED
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-
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iii
TABLE OF CONTENTS
ABSTRAC';. - e s e . * Q.‘. . . * .I '- L » * . * - . * “ e - . .
INTRODUCT ION * - » * * . * -, .' . - * * - » * - * * * e . - [ -
-y
JE
(‘fl)
PREDICTIONS BEFORE MSRE OPERATION - . « . . . . .
OBSERVATIONS DURING MSRE OPERATION . . . . . . .
1
2
PROCESSES AFFECTING 1®*XE IN MOLTEN-SALT REACTORS . . . . . . 3
| 6
7
DEVELOPMENT OF MATHEMATICAL MODELS OF MSRE 3*°XE
- DISTRIBUTION
COVER-GAS BEHAVIOR . . v ¢ ¢ o o o o o + o 30
ANALYSIS OF MSRE COVER GAS AND '*°XE BEHAVIOR . 51
DISCUSSION OF RESULTS . & « & o o s « o o o + 91
CONCLUSIONS v & o v o o o o oo o o v o o s o 95
ACKNOWLEDGMENT . &+ v oo o o oo o o o o o o « 97
REFERENCES « o+ « o o o o s s o o o o o o 0 s 0. 98
APPENDIX « « o o o e o v o o o m o oo o e u 101
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XENON BEHAVIOR IN THE MOLTEN SALT REACTOR EXPERIMENT.
*
J. R. Engel. R. C. Steffy
ABSTRACT
Since molten salt reactors are based on a circulating fluid fuel, the
possibility exists for continuous removal of ***Xe (by gas-liquid con-
tacting) as a means of impréving their breeding performance. A reasonably
detailed understanding of the xenon behavior in such reactors is essential
for accurate prediction of the removal capability. The xenon poisoning
in the Molten Salt Reactor Experiment (MSRE) was ‘extensively studied in
an effort to develop an understanding of the behavior mechanisms. .
Xenon poisoning calculations made prior to ‘the operation of the MSRE
were based on a mathematical model that neglected any effects of cover-gas
solubility in the salt. These calculations reproduced reasonably well the
observed steady-state poisoning as a function of circulating void fraction
when an insoluble cover gas, argon, was used but they did not adequately
describe the transient behavior. In addition they did not predict the very
low xenon poisoning that was observed at low void fractions with a more
'_ soluble cover gas, helium.
A more'detailed'mathematiCal model which allowed inclusion of cover-
gas solubility effects was developed in an effort to better describe the
observed results. This model successfully described the different poison-
ing effects with helium and argon at low void fractions but it required
the use of mass transport and xenon stripping parameters that differed sig-
‘nificantly from the predicted values. These calculations also failed to
~describe adequately the transient observations. S
A comparison of calculated and observed effects suggests that 1)
- - circulating bubbles may strongly influence the transport of xenon from the
~ fluid to graphite, and 2) both the gas transport and stripping processes
may be affected by operation at power, As a consequence, additional in-
"'vestigations would be desirable to further elucidate the behavior of noble
gases in molten-salt reactor systems.
*Curtentlyrassociatediwith Tennessee Valley Authority,,Chattanooga,
Tennessee. |
INTRODUCTION
The Molten Salt Reactor Experiment (MSRE) was in nuclear operation
from June 1, 1965 to December 12, 1969. During that time the reactor
generated 13,172 equivalent fullpower hours of energy at power levels up
to 7.4 Mw. The reactor system and the overall operéting experience have
been extensively described in the open literature. (Refs. 1 - 4). This
report deals with a specific aspect of that experience, the behavior of
xenon-135. 7 ,.~., - o
Because the fuel is é circulating fluid, the mobility of all the fuel
constituents, including the fiésion products, is an important cpnsideratidn
in the.overall performancé of molten-salt systems. This mobility is
espécially important for the noble-gas fission products because they,:‘
typically, have very low solubilities in molten salts and because some,
~ notably '*°Xe, are significant neutron absorbers. Thus, the potential for
continuous and rapid removal of the gaseous fission products offers the
possibility of reducing both the circulating fission-product inventory and
the neutron losses to ?”Xe.* Although neither of these considerations was
of major significance in the MSRE,. the behavior of '*°Xe was studied ex-
tensively in an effort to develop an understanding of the mechanisms in-
volved. Such an understanding is essential to the reliable prediction of
xenon behavior in other MSR designs. | -
The purpose of this report is to provide a basis for discussion and
then to describe the xenon behavior observed in the MSRE. Since.signifi-
cant differences were found when different cover gases (helium or argon)
were used for the salt, this aspect of the behavior will receive consider-
able attention, We then develop a mathematical model and discuss the re~
sulté of parametric studies whose.objective waé a consistentrdeséription
of all the observed phenomena. Finally some conclusions are drawn about
the apparent xenon behavior and suggestions are offered for experimental
investigations that may further elucidate this behavior.
% : ’ '
Calculations for large molten salt reactors indicate that a '*°Xe
poison fraction around 0.5% is desirable for good breeding performance.
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PROCESSES AFFECTING '®°Xe IN MOLTEN-SALT REACTORS
Although many of the xenon behavior processes are the same in a molten
salt reactor as in any other reéctor, the'fact that the fuel is not con-
fined within discrete, impervious elements in the core introduces some
significant differences. The basic procesées for production and removal
of '®*°Xe are outlined in Fig. 1.
The majority of the !23Xe that is produced results from the decay of
the 6.7-hr half-1ife precursor '*?I, At least some of this iodine is pro-
duced by the decay of '®*°Te whose behavior in molten-salt systems is not
completely defined.5 Howe#er, because of its short (29 sec) half-life, Te
has very little effedt/on'th57135’chain. Thus, since iodine has essentialiy
no tendency to leave the salf;s the '®°Xe that is pfoduced directly from
'3%1 is formed in the circulating salt, at a uniform rate around the entire
fuel loop. As indicated on Fig. 1, only about 70% of the '®°I decays lead
directly to '°°Xe and the remainder produce the metastable form, *°>"Xe.
Although the occurrenceiof”this'isomer is unimportant in reactors where all
the fission products are confined within fuel elements, it has potential
significance in fluid fuel systems, particularly if there are other xenon
behavior mechanisms with time constants that are short relative to the
16-min. half-life of the isomer. (Fig. 1 indicatéS—one'such.mechanismé
transfer from the fuel salt into the offgas system. Not shown, but also
possible, is tfansport into the graphite poresQ) The significance of the
16-minute isomerhis.also_SOmQWhat dependent on its neutron absorption
cross section. Although there are no data available on ;he Cross seétion
of '°°™Xe (Ref. 7), it is,preéfimed'tb'befinegligible-in comparison to that
of 1-MXF.!-.
‘The '3%Xe that is fibt produced by the iodine decay scheme is produced
directly from fission; Literature reports of the fractibn_of'theftotal
13%Xe yield that is produced_directly'in 233y fission range from 3.8%
(Ref. 8) to 18% (Ref. 9). This fraction would be expected to have alfiost
~ no effect on steady-state xenon poisoning but it could significantly\af-
fect the transient behavior following major changes in power level.
tor.
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| : 3257/’\\\ ’//,/’TEE?'
| 12350, B 135 B 70% 135, _
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Fig. 1. Processes Affecting Xenon Poisoning in a Molten-Salt Reac-
ORNL-DWG 71-8031
FUEL
SALT
+n__ 136 Xe
25 | | srapmiTE
Xe g | PORES
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1353
Once the Xe has been formed, it is subject to the same decay and
neutron absorption processes as in any other reactor. Some difference is
‘introduced by the fact thattxendn in the circulating fluid is exposed to a
differentraverage neutren,flux than the xenon in the graphite. However, a
- more important complication is the additional path for xenon removal by
stripping into the offgas ayStem. The reduction in xenon poisoning that
can be achieved depends upoa the extent to which stripping can be made to
compete_fiith the other 1oas&tetms, _In principle, xenon can either be
stripped directly from the citculating_salt into the offgas or it can
transfer to‘circu;ating,bubbles and be removed by a bubble exchange pro-
cess. Thus, the detaills of these two precesses, as well as the rate of
xenon mass transfer between bubbles and liquid are important in describing
.the overall xenon behaVior;t,In addition, any xenon that is transported to
the unclad graphite must be dealt with separately because the xenon inven-
tory in the graphite is.notlavailable for stripping. This process depends
upon the mass transfer from the fluid to the graphite surface and on the
porosity (storage volume) and permeability (accessibility of that volume)
. of the graphite itself.
Another mechanism of potential significance is an abnormal out-of-
- core holdup of xenon, either in_gas-pockets or.on solid surfaces. Opera-
tion of the MSRE showed that there were no significant gas pockets in the
loop except at the reactor access nozzle and the gas exchange with that
region appeared to be too slow to exert much influence on xenon. Holdup
in corrosion-product scales was shown to be significant in an aqueous sys-
~ tem!® because of iodine'adéetption on the scale. ,However, there was no
corrosion?product scalefih_thefiMSREfand no tendency for iodine to leave
the salt. Xenon sorption on surface active particles that are held out
t'of circulatiqn (possibly in foam in the pump bowl) may also be possible
but will not be considered in this analysis.
PREDICTIONS BEFORE MSRE OPERATION
Aécurate description of the xenon behavior in the MSRE was an éarly
objective of the project so a considerable part of the reactor development
effort was directed toward this goal The fuel circulating pfimp was ex-
tensively tested in both water'® and molten-salt?? loops to evaluate its
hydraulic characteristics, gas stripping and cover-gas entrainment,
Additional gas stripping tests were performed on a mockup.?® A full scale
water mockup of the reactdr vessel was used to study coté'flbw'pattérns,’“
partly as an aid to evaluating mass transfer processes in the loop. The
MSRE graphite was subjected to a variety of tests'®s® some of which pro-
~ vided data on porosity and permeability which were directly applicable to
the xenon problem. To support these separate studies, an experiment was
performed with the MSRE, prior to nuclear operation, in which krypton was
“injected into'the system and then purged out.!’ The objective of all this
‘work was to provide sufficient data on tfie various mechanisms so that rea-
' sonable predictions could be made of the xenon poisoning.
A mathematical model was constructed to use the available 1nformation
to predict steady-state *>*Xe poisoning in the 'MSRE.!” Since ‘the development
" tests had indicated that there would be a significant fraction of undis-
solved cover gas (1 to 2 vol. %) circulating with the salt, this model in-
cluded the mass transfer of xenon between salt and bubbles and the effects
of bubble stripping. However, early operation of the MSRE with molten
salt indicated that there would be essentially no circulating bubbles
18 Consequently, xenon poisoning cal-
under normal operating conditionms.
culations were made for a variety of circulating void fractions, including
zero. ' r
| In addition to the treatment of circulating voids, several other
apptoximations and assumptions made for this model are ifiportant.' The
solubility of the reactor cover gas (helium) in molten salt was neglected.
With this assumption it was then quite reasonable to treat the entire fuel
loop as a singie well-stirred tank. The production of ®°Xe was assumed
to be uniform around the loop and was confined to the salt phase. That is,
formation by decay of **°UXe was neglected and the direct fission yield
£
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was combined with the iodine decay term. Since only steady-state condi-
tions were considered, this simplification had almost no effect on the
results. Xenon distribution-in the graphite and the resultant poisoning
were treated in a detailed'(72 region) nuclear model of the core that also
included the radial xenon distribution within individual graphite bars.
However, mass transfer of xenon to the graphite was assumed to occur only
from the salt; direct transfer from bubbles to graphite was not allowed.
The parameter values used and the results obtained from calculations
'with this model are described in detail in Ref. 17. Figure 2 shows one
set of results in which the circulating void fraction was treated as an
independent variable. This figurerillustrates the monotonic decrease in
poisoning with increasing uoid fraction that wasbtypical'of the results
obtained. (Note that in Figure 2 the xenon poisoning is in terms of
233y, Subse-
poison fraction, neutron absorptions in lssXe/absorption in
quent results will use the Xenon reactivity effect, % Sk/k, since this
can be compared more readily with measured values. For the MSRE, the re-
‘activity effect of.a poison‘was approximately 0.8 times the poison
fraction.)
OBSERVATIONS DURING MSRE OPERATION
The behavior of xenon in the MSRE was observed throughout the opera-
tion of the reactor. The primary tool for these observations was the sys-—
19,20
tem reactivity balance’ which was calculated every 5 min by an on-line
computer while the reactor was in operation. This. computation was devel-
oped to provide a real-time monitor of the reactor system for unexpected
'changes in nuclear reactivity. It included calculations of all the known
reactivity changes from'a.reference state as functions of time, temperature,
| power, and fuel loading. All'the'calculated effects, along with the ob-
'served control-rod poisoning were summed and any deviation from zero could
be regarded either as an anomaly or an error in one or more of the calcu-
lated terms. Initially, the only large term in the reactiv1ty balance
with a-significant-uncertainty was the xenon poisoning. _Subsequently, the
accuracy of the other terms was shown by results at zero power with no
ORNL-DWG 67-1973
BUBBLE STRIPPING EFFICIENCY (%)
0o
138%e POISONING (%)
o 0.25 0.50 075 1.00 1.25
MEAN BUBBLE CIRCULATING VOID (%)
Fig. 2. Predicted !3%Xe Poison Fraction in the MSRE with Circulating
Bubbles at 7.5 MW(t).
(w
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2° This information, along with other evidence that no
xXenon present.
anomalous effects were present, allowed us to evaluate the actual xenon
poisoning not only at steady state‘but also during transients produced by
changes in the reactor-power'level and other operating parameters. During
those parts of the operation when there were no (or almost'no) circulating
voids, reactivity'balances'at power were sufficient to define the xenon
poisoning. However, when the circulating void fraction was significant,
' additional data were required'at zero power with no xenon present to permit
separation of the direct reactivity effect of the bubbles.
Although most of'thelkenon'poisoning data were extracted from
reactivity-balance results some supplementary data were obtained from
h samples of the reactor offgas. Since both *3%Xe and *®®Xe are stable
fission products with insignificant neutron absorption cross sections, a
‘comparison of the fission-yield ratio for these isotopes with the actual
isotopic'ratio in the offgas provides a measure of the neutron absorptions
in '®°%e. Such comparisons were made for several samples isolated under
steady-state conditions but the results were too scattered to contribute
significantly to the detailed analysis of xenon behavior. The results did,
however, confirm that the conclusions drawn from the reactivity balances
‘were mnot grossly in error.
Another technique_thatywasattempted'was‘direct measurement of the
‘S’XeVCOncentration:in the reactor offgas at'the fuel-pump outlet using
remote gamma—ray spectrometry. ) When the reactor was operated at high
power the radiation level from the offgas line was so high that consider-
able shielding had to be inserted between the source and detector to ob-
tain manageable pulse conntinéirateSL The effect of this Shielding on
*
the efficiency of the detector system at the energy of the principal '®°Xe
"gamma ray (249. 65 kev) introduced sufficient uncertainty to completely ob-
‘scure the results. At lower power 1evels, residual xenon ‘from previous |
ihigh—power operation had a similar effect., While this technique appears
to offer some promise for studying xenon behavior, additional development
would be required beyond that which was available on the MSRE
The introduction of shielding makes this efficiency very strongly
energy dependent below about 300 kev.
10
Circulating Voids. | \usj
Although this report is cdncerned primarily with'the behavior of
- Xenon, that behavior is so strongly affected by circulating voids that a
summary of the experience with voids is presented to prpvide a basis for
”further discussion. A detailed description of the void behavior may be
found in Ref. 21. | .
During the early operation of the MSRE, both in prenuclear tests and
the zero-power experiments, there was no evidence of circulating gas bub-
bles under normal conditions. However, voids were observed when the sys-—
tem temperature and fuel-pump level were reduced to abnormally low values.
Evidence for the presence of circulating voids began to appear after a few
months of operation at power. A series of prgssure—release tests on the
fuel loop in July_1966.confirméd that some voids were then present even at
normal system cofiditions. Various interpretations of the eariy data indi-
18’22
cated void fractions as high as 2 to 3 vol. Z%. However, as more data
1]
were obtained and evaluated we concluded that the normal void fraction in
the reactor core was quite low — in the range of 0.02 to 0.04 vol. Z.%%2°
Once it became established; the circulating void fraction remained rela- : v
tively constant throughout the ?°U operation of the reactor. Signifi-
cant variationé could, however, be induced by changes i# system tempera-
ture, overpressure, and fuel-pump level. The changes were identified.by
their reactivity effects®*® and by changes in the neutron-flux noise spec-
¢ The results of one series of void-fraction measurements based on
trum,?
reactivity effects are summarized in Table 1.. Because of uncertainties
in the absolute magnitude of the void fraction, the values shown are changes
from the minimum void fraction that was attained. In general, the void
fractions increased with decreasing temperature and increasing préssurea
Although these measfirements did not show any dependence on fuel—pump level,
the associated noise measurements indicated higher void fractions at lower
levels.
%
The entire reactor operation with®®°U fuel was carried out with -
helium cover gas and with the fuel circulating pump operating at normal, ( 7
full speed (1189 rpm). ' . \=99
")
)y
11
Table 1
Effect of Operating Conditions on Core Void Fraction
- In MSRE with *°°U Fuel?
Fuel Pump 'ReaCtdf Ofitlet
Changé from Min.
Fuei'Pump
Overpressure . = Temperature Level Range Core Void Fraction
(psig) - (in.) (Vol %)
5 1225 5.6 — 6.2 0
5 1210 5.3 ~-6.1" 10.03
5 1180 5.3 — 5.7 ' 0.11
9. 1225 5.6 — 6.2 0
9 1210 . 5.3—6.0 0.04
9 1195 . 5.3-5.9. - 0.10
9 1180 . 5.3 —5.6 ~0.18
3 1225 5.6 — 6.2 0
3 1180 5.3 —5.8 0.10
“Helium covér gas; 1189 rpm fuel-pump speed.
Based on reactivity effec
t at zero power.
12
After recovery of the ***U mixture from the fuel salt and the ad-
dition of 2°°U, the system behavior with regard to circulating voids
changed markedly: the nominal core void fraction went to 0.5 to 0.7 vol. %.
This change, along with other observations prompted a more detailed study
of the void behavior. Some early experiments indicated that, of the para-
meters available for change in:the MSRE, the circulating void fraction was
most sensitive to changes in fuel-pump speed. Consequently this approach
was used to vary the void‘fraction. Figure 3 shows the éffect of pump
speed on the void‘fractiofi for both flush and 2°*U-fuel salts with helium
and argon as the system cover gas. 'Although'we never observed circulating
voids in the flush salt (with helium cover gas) during,the-gssUrfihase of
the operatibn, this salt did develop voids with only a small increase in
fuel pump speed (to 1240 rpm). The different void fractions obtained with
helium and argon apparently reflect thé lower solubility of argon in molten
.salt. That is, for a givén rate of gas.ingestion,at the fuel pump, a
larger fraction of the argon would bé expected to remain undissolved.i The
core void fraction remained relatifiely stable aroufid‘O.S‘éoliz for most of
the 2°°U operation. However, small variations apparently did occur which
had measurable effects on the xenon poisbning; The inability to precisely
define the system void fraction under all operating conditions added con-
siderable uncertainty to the measurement of xenon poisoning as a function
of void fraction. - .
One other aspect of the behavior of.circulating'voids in the MSRE
that will be referred to later is the rate at which the circulating void
fraction could be changed, particularly in the direction of a lower value.
On several occasions, excess circulating voids were introduced by pressure-
release tests or by other system perturbations and, in every case, these
voids subsequently disappéared at a rate which indicated a bubble strip-
ping efficiency of 50 to 100% on the streams passing through the pump bowl.
i
ik g e
o)
"}
C
13
ORNL-DWG 69~ 10544
] i
SALT ~ COVER GAS
0.7— o FLUSH He
0.6
7
® FLUSH. Ar I
& FUEL He
A FUEL Ar :
/
}
o
o
)
t
LOOP VOID FRACTION (%)
o o
(8] b
8
_\‘\J
0.1 - — 7 ;' I
| .Aiéfxf/{
. 700 800 900 1000 1100
' FUEL PUMP SPEED (rpm)
Fig. 3. _Effecf of Fliel-Pmnp Speed on Void Fraction in Fuel Loop.
1300
14
Xenon Poisoning with ?°°U. Fuel -
Since the early operations at the MSRE had indicated that thére were
no circulating voids, the xenon poisoning was predicted on that basis.
Calculations using the model described above showed that, at full power |
(7.4 Mw), the poisoning would amount to about 1.08% 8k/k. When the re-
actor was first operated at power, the reactivity-balance results indicated
that the actual xenon poisohing would be much less than had been antici-
pated. At that time, attempts to use the reactivity balance as an anomaly
detector were deferred (at least during xenon transient conditions) and
the results were used to evaluate the xenon effect. Although this use of
the reactivity balance required the assumption that no anomalous effects
occurred along with the xenon changes, the experience during conditions |
of steady xenon poisoning supported its validity.
Steady-State Values
The first measurements of steady-state xenon poisoning at power levels -
of'S Mw or greater were obtained in April and May 1966. These values and
their associated power levels are listed in Table 2. On the surface, the | .
early values appear to be inconsistent because the highest power is associ-
ated with the lowest xenon value. Little significance was attached to
these differences because of the very large difference between the expected
and observed values and because we had not yet established full confidence
in the reactivity balance. The results were valid, however, and the dif-
ferences are at least.qualizatively explainable. We have already shown
that small differences in system temperature and pressure cause signifi-
cant variations in the circulating helium void fraction and will show sub-
sequeptly that, with helium cover gas, a higher core void fraction leads
to higher xenon poisoning. Both of the first two values were obtained
under conditions that tended to increase the void fraction (i.e. lower
temperaturé at 5 Mw and higher overpressure at 6.7 Mw) so it appears
likely that the different values are attributable to void-fraction vari- -
ations. This explanation is contingent upon the existence of circulating
voids which was not demonstrated until July, 1966. However, there appears ST
KfiH)
»)
L
(‘ |
15
Table 2
Early Measurements of Steady State '®*Xe Poisoning
~In MSRE with 22°U Fuel