collected 25 cm to the left and to the right of the
sphere. In each core there was onesection with a very
small amount of plutonium (0.1 and 0.03 ng). The
plutonium in the other sections was not distinguishable from background.
A Chromel-Alumel thermocouple was attached to

the side of the GIS with an epoxy adhesive. During
the winter cycle the external temperature varied

between 180 and 192°C. After the change to the
summercycle, the temperature increased to 200 to

210°C. During a rain the temperature dropped below
50°C, and when the temperature and humidity controls were shut down, resulting in air stagnation, the
temperature rose to 235°C.

5. Spallation

Induced

by

Liquid

Nitro-

gen. Earlier work has demonstrated that the airborne plutonium concentration increased

dramatically during a rain on large, thermally hot
PPO pieces. This has always been presumed to be
the result of thermal shock to the fuel’s surface,

resulting in the spallation of tiny fragments of
plutonia. We decided to find out if this cooling

mechanism was a general phenomenon,or if water
played a significantrole in the process by meansof a
chemical reaction with the hot fuel.
We conducted an experiment where

liquid

nitrogen drops fell.on chunks of PPO fuel in one of
the environmental test chambers. This liquid

nitrogen rain continued for 5 minutes. Air samples
were taken before, during, and after the rain. We

found that the airborne plutonium activity increased
by four orders of magnitude at the onset ofthe cooling period. About an hourafter the end ofthe liquid
nitrogen rain the airborne plutonium concentration
had dropped back to its prerain level of 0.1 nCi/m?.
These results are quantitatively similar to those
found with aqueous rains, and suggest that
hydrolysis reactions are not involved in the spallation process during an aqueous rain.
The air filters on which the plutonium was
collected contained a short-lived alpha activity, in

addition to the the long-lived plutonium activity.

the liquid nitrogen rain. Very little was found on the
stainless steel surface.

We also made background measurements on a

separate set of the same kinds of surfaces by exposing them to the chamberair for 48 hours before the
liquid nitrogen rain. The fact that significant
amounts of alpha activity were found on the glass

surface suggests that spontaneous spallation occurs
continually, most likely caused by radiation damage
in the plutonium oxide.
A third set of adsorber measurements was made

one dayafter the liquid nitrogen rain. These results
showed far lower adsorption rates than existed prior
to the liquid nitrogen rain. Apparently the thermal

shockof the rain not only causes a great increase in
spallation, but also frees loose particles created by

radiation damage, so that at the end of the rain a
fresh, undamaged surface is exposed.
Significant soil contamination was observedafter

the liquid nitrogen rain. The radioactivity, however,

was found only on the soil surface and not beneath
the surface. This is unlike soil contamination in the
case of aqueous rains, where some of the plutonia
particles are transported downward through thesoil

by the rainwater that drains through the soil. Thus
hydrodynamic transfer is a significant transport
mechanism under aqueousrain conditions.

III. DISSOLUTION RATES OF 7%pu0., IN
PERCHLORIC ACID
(James H. Patterson, Gilbert B. Nelson, and

George M. Matlack)

This experiment has been terminated. A topical
report has been completed and will be issued as
LASL report LA-6184.
IV. SORPTION OF PLUTONIUM BY SOILS

This short-lived activity was not present in samples

(Gilbert B. Nelson, Nicholas Vanderborgh,
George M. Matlack)

plutonia, but also radioactive gases (72°Rn and
222Rn) entrapped in the plutonium oxidecrystal lattice structure.
During this experiment we also measured the adsorption of the airborne plutonia on four different
types of surfaces: glass, Teflon, stainless steel, and
Lucite. Glass was the most effective collector of the
airborne plutonia, adsorbing approximately 1000
times more than the Teflon or Lucite surfaces during

Weare continuing the experiments to measure the
absorption of plutonium by soils. This is done by

collected prior to the rain. We believe that the thermal shock releases not only very fine particles of

and

allowing dilute plutonium to flow through soil contained in glass columns. Thefeed solution fed to the
soil columns is a dilute, neutral solution of
plutonium chloride, known to be unstable asit ages.

This type of feed solution is necessary, however, to

simulate rainwater contaminated with plutonium as

it percolates through soils.

10
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