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ORNL-4191 - the Molten Salt Energy Technologies Web Site

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The losses indicated by <strong>the</strong>se samples are ap-<br />

preciable. The mean of four samples shows nearly<br />

30 pg/sample or about 3.5 pg per cubic centimeter<br />

of helium. This would correspond to somewhat<br />

less than 20 g/day of 'U or nearly 60 g/day of<br />

<strong>the</strong> uranium in <strong>the</strong> fuel. (The figure remains at<br />

nearly one-half this level if <strong>the</strong> highest figure is<br />

rejected.) It seems absolutely certain that <strong>the</strong><br />

reactivity balances on <strong>the</strong> reactor through 250<br />

days of full-power operation would have speedily<br />

disclosed losses of far smaller magnitude than<br />

<strong>the</strong>se. It is difficult to conceive of a mechanism<br />

o<strong>the</strong>r than volatile UF6 to account for losses of<br />

uranium to <strong>the</strong> vapor. It is, however, extremely<br />

difficult to see how losses of this sort could be<br />

reconciled with <strong>the</strong> nuclear behavior (and <strong>the</strong><br />

chemical analyses) of MSRE. Fur<strong>the</strong>r samples<br />

of <strong>the</strong> gas system will be made to help resolve<br />

this apparent dilemma.<br />

The effect of short shutdown and pump stoppage<br />

(FP11-42) on noble-metal volatilization was in-<br />

significant. This suggests that <strong>the</strong> volatilization<br />

process does not depend on fuel nor bubble cir-<br />

culation nor on <strong>the</strong> fissioning process itself, but<br />

is probably a local phenomenon taking place at <strong>the</strong><br />

fuel-salt-gas interface. Beryllium additions to <strong>the</strong><br />

fuel had no discernible effect on <strong>the</strong> volatilization<br />

of noble-metal fission products. This fact is rein-<br />

forced in some detail (see subsequent sections of<br />

this chapter) by data obtained by insertion of<br />

getter wires into <strong>the</strong> pump bowl vapor space.<br />

The effect of reactor drain and long shutdown<br />

(FP12-7) was consistently to lower observed<br />

noble-metal volatilization (observed activities<br />

were, of course, calculated back to <strong>the</strong> time of<br />

previous shutdown). This observation is con-<br />

sistent with all previous data on <strong>the</strong> effect of<br />

long shutdowns. Presumably an appreciable<br />

fraction of <strong>the</strong> noble metals is deposited on <strong>the</strong><br />

walls of <strong>the</strong> drain tank and reactor system during<br />

a long shutdown. The minor effect of short shut-<br />

down and <strong>the</strong> incomplete deposition during long<br />

shutdown seem to indicate a slow deposition<br />

process.<br />

The pressure release experiment (FPll-53) re-<br />

sulted in an appreciable increase of volatilization<br />

of most fission products but not of "Mo or 132Te.<br />

Niobium-95 showed <strong>the</strong> most distinct increase. It<br />

is particularly puzzling that <strong>the</strong> '' 'Te concentra-<br />

tion increased markedly while <strong>the</strong> ' 32 Te concen-<br />

tration fell slightly. Clearly, fur<strong>the</strong>r experiments<br />

119<br />

of this kind would be required to permit definite<br />

interpretations.<br />

It cannot be claimed that <strong>the</strong> mechanism for<br />

volatilization of many of thcse materials is known.<br />

As has been shown elsewhere' f2 <strong>the</strong> volatile flu-<br />

orides of many of <strong>the</strong>se materials (notably Mo, Ru,<br />

Te, and, probably, Nb) are too unstable to exist<br />

as equilibrium components of a fuel system con-<br />

taining appreciable quantities of UF3. It is true<br />

that, for example, "Mo formed at about 5 x 10"<br />

atoms/day probably exceeds greatly <strong>the</strong> solubility<br />

limit for this material in <strong>the</strong> salt. Since it is born<br />

in <strong>the</strong> salt in an atomic dispersion, it may, in ef-<br />

fect, behave as a supersaturated solution; that is,<br />

<strong>the</strong> activity of molybdenum may, in fact, be mark-<br />

edly greater than unity. It seems most unlikely<br />

that it can have activities greater than 10- lo,<br />

which would be required if MoF, were to be stable.<br />

Such Eindings as <strong>the</strong> presence of l1 Ag, for which<br />

it is difficult to imagine volatile fluorides, seem<br />

to render <strong>the</strong> volatile fluoride mechanism more un-<br />

likely. It still seems more likely that an ex-<br />

planation based upon <strong>the</strong> finely divided metallic<br />

state will prove iruc?, though such explanations<br />

also have <strong>the</strong>ir drawbacks.<br />

9.2 FISSiON PRODUCTS IN MSRE FUEL<br />

The program of sampling and analysis of samples<br />

of MSRE fuel for fission product species has been<br />

continued by use of apparatus and techniques de-<br />

scribed previously. '-' Table 9.2 shows data for<br />

16 fission product isotopes and for 23 'Np obtained<br />

from a series of four samples from a long stable<br />

run of MSRE, from a sample obtained shortly after<br />

shutdown in this run, a sample after <strong>the</strong> salt had<br />

been cooled for 42.5 days, and a sample from a<br />

relatively early stage in <strong>the</strong> subsequent power run.<br />

Captions in this table show <strong>the</strong> operating history<br />

of MSRE and <strong>the</strong> special conditions prevailing in<br />

<strong>the</strong> reactor at <strong>the</strong> time <strong>the</strong> sample was taken.<br />

Table 9.2 also includes estimates of <strong>the</strong> fraction<br />

of <strong>the</strong> isotope represented by <strong>the</strong>se analyses in<br />

<strong>the</strong> 4850 kg of circulating fuel.<br />

'5. S. Kirslis and F. F. Blankerrship, Reactor Cham.<br />

Div. Ann. Progr. Rept. Dec. 31, 1966, <strong>ORNL</strong>-4076, p.<br />

48.<br />

3S. S. Kiislis arid F. F. Blankenship, MSR Program<br />

Serninnn. Progr. Rept. Feh. 28, .1967, <strong>ORNL</strong>-4119, p.<br />

124.

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