Natural nuclear fission reactor

File:Gabon Geology Oklo.svg

Geological Situation in Gabon leading to natural nuclear fission reactors
1. Nuclear reactor zones
2. Sandstone
3. Uranium ore layer
4. Granite

A natural nuclear fission reactor is a uranium deposit where analysis of isotope ratios has shown that self-sustaining nuclear chain reactions have occurred. The existence of this phenomenon was discovered in 1972 by French physicist Francis Perrin. The conditions under which a natural nuclear reactor could exist were predicted in 1956 by P. Kuroda. The conditions found at Oklo were very similar to what were predicted.

At the only known location, three ore deposits at Oklo in Gabon, sixteen sites have been discovered so far at which self-sustaining nuclear fission reactions took place approximately 1.5 billion years ago, and ran for a few hundred thousand years, averaging 100 kW of power output during that time.

History

In May 1972 at the Pierrelatte uranium enrichment facility in France, routine mass spectrometry comparing UF₆ samples from the Oklo Mine, located in Gabon, Central Africa, showed a discrepancy in the amount of the ²³⁵U isotope. Normally the concentration is 0.7202%; these samples had only 0.7171% – a significant difference. This discrepancy required explanation, as all uranium handling facilities must meticulously account for all fissionable isotopes to assure that none are diverted for weapons purposes. Thus the French Commissariat à l'énergie atomique (CEA) began an investigation. A series of measurements of the relative abundances of the two most significant isotopes of the uranium mined at Oklo showed anomalous results compared to those obtained for uranium from other mines. Further investigations into this uranium deposit discovered uranium ore with a ²³⁵U to ²³⁸U ratio as low as 0.440%. Subsequent examination of other isotopes showed similar anomalies, such as Nd and Ru as described in more detail below.

This loss in ²³⁵U is exactly what happens in a nuclear reactor. A possible explanation therefore was that the uranium ore had operated as a natural fission reactor. Other observations led to the same conclusion, and on September 25 1972, the CEA announced their finding that self-sustaining nuclear chain reactions had occurred on Earth about 2 billion years ago. Later, other natural nuclear fission reactors were discovered in the region.

Fission product isotope signatures

Nd

Neodymium and other elements were found with isotopic compositions different from what is customarily found on Earth. For example, natural neodymium contains 27% ¹⁴²Nd; the Nd at Oklo contained less than 6% but contained more ¹⁴³Nd. Subtracting the natural isotopic Nd abundance from the Oklo-Nd, the isotopic composition matched that produced by the fissioning of ²³⁵U.

File:Neodynium isotope signatures.svg

A diagram showing the isotope signatures of natural neodymium and fission product neodymium from U-235 which had been subjected to thermal neutrons. Note that the Ce-142 (a long lived beta emitter) has not had time to decay to Nd-142 over the time since the reactors stopped working.

Ru

Similar investigations into the isotopic ratios of ruthenium at Oklo found a much higher ⁹⁹Ru concentration than expected (27-30% vs. 12.7%). This anomaly could be explained by the decay of ⁹⁹Tc to ⁹⁹Ru. In the bar chart below the normal natural isotope signature of ruthenium is compared with that for fission product ruthenium which is the result of the fission of ²³⁵U with thermal neutrons. It is clear that the fission ruthenium has a different isotope signature. The level of ¹⁰⁰Ru in the fission product mixture is low because of a long lived (half life = 10¹⁹ years) isotope of molybdenum. On the time scale of when the reactors were in operation very little decay to ¹⁰⁰Ru will have occurred.

File:Ruthenium isotope signatures.svg

A diagram showing the isotope signatures of natural ruthenium and fission product ruthenium from U-235 which had been subjected to thermal neutrons. Note that the Mo-100 (a long lived double beta emitter) has not had time to decay to Ru-100 over the time since the reactors stopped working.

Mechanism of the reactors

The natural nuclear reactor formed when a uranium-rich mineral deposit became inundated with groundwater that acted as a neutron moderator, and a nuclear chain reaction took place. The heat generated from the nuclear fission caused the groundwater to boil away, which slowed or stopped the reaction. After cooling of the mineral deposit, short-lived fission product poisons decayed, the water returned and the reaction started again. These fission reactions were sustained for hundreds of thousands of years, until a chain reaction could no longer be supported.

Fission of uranium normally produces five known isotopes of the fission-product gas xenon; all five have been found trapped within novel aluminium foams in the remnants of the natural reactor, in varying concentrations. The concentrations of xenon isotopes, found trapped in mineral formations 2 billion years later, make it possible to calculate the specific time intervals of reactor operation: approximately 2 hours and 30 minutes.

A key factor that made the reaction possible was that, at the time the reactor went critical, the fissile isotope ²³⁵U made up about 3% of the natural uranium, which is comparable to the amount used in some of today's reactors. (The remaining 97% was non-fissile ²³⁸U.) Because ²³⁵U has a shorter half life than ²³⁸U, and thus decays more rapidly, the current abundance of ²³⁵U in natural uranium is about 0.7%. A natural nuclear reactor is therefore no longer possible on Earth.

The Oklo uranium ore deposits are the only known in which natural nuclear reactors existed. Other rich uranium ore bodies would also have had sufficient uranium to support nuclear reactions at that time, but the combination of uranium, water and physical conditions needed to support the chain reaction was unique to the Oklo ore bodies.

Another factor which probably contributed to the start of the Oklo natural nuclear reactor at 2 billion years, rather than earlier, was the increasing oxygen content in the earth's atmosphere. Uranium is naturally present in the rocks of the earth, and the abundance of fissionable ²³⁵U was at least 3% or higher at all times prior to reactor startup. However, uranium is soluble in water only in the presence of oxygen. Therefore, the rising oxygen levels during the aging of earth may have allowed uranium to be dissolved and transported with groundwater to places where a high enough concentration could accumulate to form rich uranium ore bodies. Without the new aerobic environment available on earth at the time, these concentrations probably couldn't have taken place.

It is estimated that secondary enrichment of the uranium in centimeter- to meter-sized veins consumed about six tons of ²³⁵U and elevated temperatures to a few hundred degrees Celsius. Remarkably, the non-volatile fission products have only moved a few centimeters in the veins during the last 1.5 billion years. This offers a case study of how radioactive isotopes migrate through the earth's crust—a significant area of controversy as opponents of geologic nuclear waste disposal fear that releases from stored waste could end up in water supplies or be carried into the environment.

Relation to the atomic fine-structure constant

The natural reactor of Oklo has been used to check if the atomic fine-structure constant <math>\alpha</math> might have changed over the past 2 billion years. That is because <math>\alpha</math> influences the rate of various nuclear reactions. For example, ¹⁴⁹Sm captures a neutron to become ¹⁵⁰Sm, and since the rate of neutron capture depends on the value of <math>\alpha</math>, the ratio of the two samarium isotopes in samples from Oklo can be used to calculate the value of <math>\alpha</math> from 2 billion years ago.

Several studies have analysed the relative concentrations of radioactive isotopes left behind at Oklo, and most (but not all) have concluded that nuclear reactions then were much the same as they are today, which implies alpha was the same too.

In fiction

In Manifold: Space by Stephen Baxter, a far-future feudalist society exploits a naturally occurring fission reactor for power.

External links

• The natural nuclear reactor at Oklo: A comparison with modern nuclear reactors
• Oklo Fossil Reactors
• Yucca Mountain Project: Oklo:Natural Nuclear Reactors

• Oklo. Fission reactors on the Earth
• NASA, Astronomy Picture of the day: Oklo, Fossile Reactor, Zone 15

References

• Andrew Karam, The natural nuclear reactor at Oklo, Radiation Information Network, April 2005, [1]
• W. Miller et al.: Geological Disposal of Radioactive Wastes and Natural Analogues. ISBN 0-08-043852-0, PERGAMON (2000)
• Gauthier-Lafaye, et al.: Natural fission reactors in the Franceville Basin, Gabon: a review of the conditions and results of a "critical event" in a geologic system, Geochim. Cosmochim. Acta, 60, 48314852, 1996.
• Neuilly, M.et al.: Sur l'existence dans un passé reculé d'une réaction en chaîne naturelle de fissions, dans le gisement d'uranium, C. R. Acad. Sci., 275D, 1847, 1972.
• Raffenach, J. C., Menes, J., Devillers, C., Lucas, M. and Hagemann, R. (1976). Études chimiques et isotopiques de l’uranium, du plomb et de plusieurs produits de fission dans un échantillon de minéral du réacteur naturel d’Oklo. Earth Planet. Sci. Lett. 30, 94)108.
• R. Bodu, H. Bouzigues, N. Moin and J.P. Pfiffelman (1971). "Sur l'existence d'anomalies isotopiques rencontrées dans l'uranium du Gabon". Comp. Rendus Acad. Sci. Paris. 275: 1731.CS1 maint: Multiple names: authors list (link)