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Investigation of the Environmental Fate of Tritium in the Atmosphere

Investigation of the Environmental Fate of Tritium in the Atmosphere

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INVESTIGATION OF THE ENVIRONMENTAL FATE OF TRITIUM IN THE ATMOSPHERE<br />

2.0 SOURCES AND CHEMICAL FORMS OF TRITIUM<br />

This section outl<strong>in</strong>es <strong>the</strong> sources and chemical forms <strong>of</strong> tritium <strong>in</strong> <strong>the</strong> atmosphere.<br />

Both natural and anthropogenic sources <strong>of</strong> tritium are described.<br />

2.1 Chemical Forms<br />

<strong>Tritium</strong> is a rare but natural isotope <strong>of</strong> hydrogen (H), and is <strong>the</strong> only natural hydrogen isotope<br />

that is radioactive. Whereas <strong>the</strong> common hydrogen nucleus conta<strong>in</strong>s a s<strong>in</strong>gle proton, <strong>the</strong><br />

nucleus <strong>of</strong> a tritium atom also conta<strong>in</strong>s two neutrons (ANL, 2005). Thus, <strong>the</strong> mass <strong>of</strong> a<br />

tritium atom is 3 times that <strong>of</strong> an ord<strong>in</strong>ary hydrogen atom. The tritium atom is sometimes<br />

designated T to dist<strong>in</strong>guish it from <strong>the</strong> common lighter isotope.<br />

Notwithstand<strong>in</strong>g <strong>the</strong> difference <strong>in</strong> mass, tritium can be found <strong>in</strong> <strong>the</strong> same chemical forms<br />

as hydrogen. The most important forms, from <strong>the</strong> perspective <strong>of</strong> atmospheric behaviour <strong>of</strong><br />

tritium, are tritiated hydrogen gas (HT) and tritiated water (HTO). These tritiated forms<br />

behave chemically like hydrogen gas (H2) and water (H2O). When tritium is <strong>in</strong>corporated<br />

<strong>in</strong>to hydrocarbon molecules with<strong>in</strong> an organism, it is referred to as organically bound tritium<br />

(OBT). S<strong>in</strong>ce OBT is not <strong>in</strong>volved <strong>in</strong> atmospheric processes, it is not considered fur<strong>the</strong>r <strong>in</strong><br />

this review. Tritiated methane (CH3T) accounts for a small amount <strong>of</strong> atmospheric tritium.<br />

2.2 Natural Abundance<br />

Hydrogen is <strong>the</strong> most abundant element <strong>in</strong> <strong>the</strong> universe, compris<strong>in</strong>g approximately 90%<br />

<strong>of</strong> <strong>the</strong> lum<strong>in</strong>ous universe by weight. Ord<strong>in</strong>ary hydrogen ( 1 H) accounts for greater than<br />

99.985% <strong>of</strong> all naturally-occurr<strong>in</strong>g hydrogen, whereas deuterium ( 2 H) comprises<br />

approximately 0.015%. By comparison, tritium ( 3 H) represents only approximately<br />

10 -16 percent <strong>of</strong> hydrogen naturally occurr<strong>in</strong>g (Gross et al., 1951).<br />

Natural atmospheric hydrogen has been estimated to conta<strong>in</strong> approximately 4 x 10 -15<br />

tritium atoms per hydrogen atom, whereas hydrogen <strong>in</strong> natural surface waters conta<strong>in</strong>s<br />

approximately 10 -18 tritium atoms per hydrogen atom, accord<strong>in</strong>g to early surveys (Bibron,<br />

1963; Falt<strong>in</strong>gs and Harteck, 1950; Fireman and Rowland, 1961; Grosse et al., 1951,1954;<br />

Harteck, 1954; Harteck and Falt<strong>in</strong>gs, 1950). On this basis, <strong>the</strong> ‘tritium unit’ (TU) was<br />

def<strong>in</strong>ed as 1 tritium atom per 10 18 atoms <strong>of</strong> hydrogen (Gross et al., 1951). Today, tritium<br />

levels are more commonly reported <strong>in</strong> activity units <strong>of</strong> Bq per litre <strong>of</strong> water, where 1 TU<br />

is equivalent to 0.118 Bq/L (e.g., ICRU, 1963).<br />

<strong>Tritium</strong> levels present <strong>in</strong> <strong>the</strong> atmosphere (T/H ratio) are approximately 10 3 to 10 4 times<br />

higher than <strong>in</strong> precipitated ra<strong>in</strong>water, although hydrogen gas quantities <strong>in</strong> <strong>the</strong> atmosphere<br />

are 10 4 -fold lower than <strong>the</strong> mean quantity <strong>of</strong> water vapour (Begemann, 1962; Bibron, 1963;<br />

Grosse et al., 1954; Harteck, 1954; Harteck and Falt<strong>in</strong>gs, 1950). Global levels correspond<br />

to approximately 0.12% <strong>of</strong> natural tritium <strong>in</strong> <strong>the</strong> form <strong>of</strong> hydrogen gas, approximately 0.1%<br />

as water vapour and <strong>the</strong> rema<strong>in</strong><strong>in</strong>g 99.78% <strong>in</strong> <strong>the</strong> hydrosphere, predom<strong>in</strong>antly <strong>in</strong> <strong>the</strong> oceans<br />

(Begemann, 1962; Jacobs, 1968). Of <strong>the</strong> total natural tritium <strong>in</strong>ventory, almost 99% has been<br />

estimated to occur <strong>in</strong> <strong>the</strong> oceans, with less than 1% occurr<strong>in</strong>g <strong>in</strong> <strong>the</strong> atmosphere and <strong>in</strong> <strong>the</strong><br />

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