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Natural nuclear fission reactor - Wikipedia
Natural nuclear fission reactor
A natural nuclear fission reactor is a uranium deposit where self-sustaining nuclear chain
reactions occur. The idea of a nuclear reactor existing in situ within an ore body moderated by
groundwater was briefly explored by Paul Kuroda in 1956.[1] The existence of an extinct or fossil
nuclear fission reactor, where self-sustaining nuclear reactions occurred in the past, was
established by analysis of isotope ratios of uranium and of the fission products (and the stable
daughter nuclides of those fission products). The first discovery of such a reactor happened in 1972
in Oklo, Gabon, by researchers from the French Alternative Energies and Atomic Energy
Commission (CEA) when chemists performing quality control for the French nuclear industry
235
noticed sharp depletions of fissile U in gaseous uranium hexafluoride made from Gabonese ore.
Oklo is the only location where this phenomenon is known to have occurred, and consists of 16
sites with patches of centimeter-sized ore layers. There, self-sustaining nuclear fission reactions
are thought to have taken place approximately 1.7 billion years ago, during the Statherian period of
the Paleoproterozoic. Fission in the ore at Oklo continued off and on for a few hundred thousand
years and probably never exceeded 100 kW of thermal power.[2][3][4] Life on Earth at this time
consisted largely of sea-bound algae and the first eukaryotes, living under a 2% oxygen
atmosphere. However, even this meager oxygen was likely essential to the concentration of
uranium into fissionable ore bodies, as uranium dissolves in water only in the presence of oxygen.
Before the planetary-scale production of oxygen by the early photosynthesizers groundwater-
moderated natural nuclear reactors are not thought to have been possible.[4]
Discovery of the Oklo fossil reactors
In May 1972, at the Tricastin uranium enrichment site at Pierrelatte, France, routine mass
spectrometry comparing UF6 samples from the Oklo mine showed a discrepancy in the amount of
235 235
the U isotope. Where the usual concentrations of U were 0.72% the Oklo samples showed
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only 0.60%. This was a significant difference—the samples bore 17% less U than expected.[5]
This discrepancy required explanation, as all civilian uranium handling facilities must
meticulously account for all fissionable isotopes to ensure that none are diverted into the
construction of unsanctioned nuclear weapons. Further, as fissile material is the reason for mining
uranium in the first place, the missing 17% was also of direct economic concern.
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Geological situation in Gabon leading to
natural nuclear fission reactors
1. Nuclear reactor zones
2. Sandstone
3. Uranium ore layer
4. Granite
Thus, the French Alternative Energies and Atomic Energy Commission (CEA) began an
investigation. A series of measurements of the relative abundances of the two most significant
isotopes of uranium mined at Oklo showed anomalous results compared to those obtained for
uranium from other mines. Further investigations into this uranium deposit discovered uranium
235
ore with a U concentration as low as 0.44% (almost 40% below the normal value). Subsequent
examination of isotopes of fission products such as neodymium and ruthenium also showed
anomalies, as described in more detail below. However, the trace radioisotope 234U did not deviate
significantly in its concentration from other natural samples. Both depleted uranium and
reprocessed uranium will usually have 234U concentrations significantly different from the secular
equilibrium of 55 ppm 234U relative to 238U. This is due to 234U being enriched together with 235U
and due to it being both consumed by neutron capture and produced from 235U by fast-neutron-
induced (n,2n) reactions in nuclear reactors. In Oklo, any possible deviation of 234U concentration
present at the time the reactor was active would have long since decayed away. 236U must have
also been present in higher-than-usual ratios during the time the reactor was operating, but due to
its half-life of 2.348 × 107 years being almost two orders of magnitude shorter than the time
elapsed since the reactor operated, it has decayed to roughly 1.4 × 10−22 its original value and
below any abilities of current equipment to detect.
235
This loss in U is exactly what happens in a nuclear reactor. A possible explanation was that the
uranium ore had operated as a natural fission reactor in the distant geological past. Other
observations led to the same conclusion, and on 25 September 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.[4]
Nd 143 144 145 146 148 150
C/M 0.99 1.00 1.00 1.01 0.98 1.06
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Fission product isotope signatures
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Isotope signatures of natural neodymium and fission product neodymium from U
which had been subjected to thermal neutrons.
Neodymium
The neodymium found at Oklo has a different isotopic composition to that of natural neodymium:
142 142
the latter contains 27% Nd, while that of Oklo contains less than 6%. The Nd is not produced
142
by fission; the ore contains both fission-produced and natural neodymium. From this Nd
content, we can subtract the natural neodymium and gain access to the isotopic composition of
235 143 145
neodymium produced by the fission of U. The two isotopes Nd and Nd lead to the
144 146
formation of Nd and Nd by neutron capture. This excess must be corrected (see above) to
obtain agreement between this corrected isotopic composition and that deduced from fission
yields.
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Ruthenium
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Isotope signatures of natural ruthenium and fission product ruthenium from U
100
which had been subjected to thermal neutrons. The Mo (an extremely long-lived
100
double beta emitter) has not had time to decay to Ru in more than trace
quantities over the time since the reactors stopped working.
99
Similar investigations into the isotopic ratios of ruthenium at Oklo found a much higher Ru
concentration than otherwise naturally occurring (27–30% vs. 12.7%). This anomaly could be
99 99
explained by the decay of Tc to Ru. In the bar chart, the normal natural isotope signature of
ruthenium is compared with that for fission product ruthenium which is the result of the fission of
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U with thermal neutrons. The fission ruthenium has a different isotope signature. The level of
100
Ru in the fission product mixture is low because fission produces neutron rich isotopes which
100
subsequently beta decay and Ru would only be produced in appreciable quantities by double
beta decay of the very long-lived (half-life 7.1 × 1018 years) molybdenum isotope 100Mo. On the
100
timescale of when the reactors were in operation, very little (about 0.17 ppb) decay to Ru will
have occurred. Other pathways of 100 99 99
Ru production like neutron capture in Ru or Tc (quickly
followed by beta decay) can only have occurred during high neutron flux and thus ceased when the
fission chain reaction stopped.
Mechanism
The natural nuclear reactor at Oklo formed when a uranium-rich mineral deposit became
inundated with groundwater, which could act as a moderator for the neutrons produced by nuclear
fission. A chain reaction took place, producing heat that caused the groundwater to boil away;
without a moderator that could slow the neutrons, however, the reaction slowed or stopped. The
reactor thus had a negative void coefficient of reactivity, something employed as a safety
mechanism in human-made light water reactors. After cooling of the mineral deposit, the water
returned, and the reaction restarted, completing a full cycle every 3 hours. The fission reaction
cycles continued for hundreds of thousands of years and ended when the ever-decreasing fissile
materials, coupled with the build-up of neutron poisons, no longer could sustain a chain reaction.
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Fission of uranium normally produces five known isotopes of the fission-product gas xenon; all
five have been found trapped 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 30
minutes of criticality followed by 2 hours and 30 minutes of cooling down (exponentially
decreasing residual decay heat) to complete a 3-hour cycle.[6] Xenon-135 is the strongest known
neutron poison. However, it is not produced directly in appreciable amounts but rather as a decay
product of iodine-135 (or one of its parent nuclides). Xenon-135 itself is unstable and decays to
caesium-135 if not allowed to absorb neutrons. While caesium-135 is relatively long lived, all
caesium-135 produced by the Oklo reactor has since decayed further to stable barium-135.
Meanwhile, xenon-136, the product of neutron capture in xenon-135 decays extremely slowly via
double beta decay and thus scientists were able to determine the neutronics of this reactor by
calculations based on those isotope ratios almost two billion years after it stopped fissioning
uranium.
Change of content of Uranium-235 in natural
uranium; the content was 3.65% 2 billion years
ago.
A key factor that made the reaction possible was that, at the time the reactor went critical
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1.7 billion years ago, the fissile isotope U made up about 3.1% of the natural uranium, which is
238
comparable to the amount used in some of today's reactors. (The remaining 96.9% was U and
235
roughly 55 ppm 234U, neither of which is fissile by slow or moderated neutrons.) Because U has
238 235
a shorter half-life than U, and thus decays more rapidly, the current abundance of U in
natural uranium is only 0.72%. A natural nuclear reactor is therefore no longer possible on Earth
without heavy water or graphite.[7]
The Oklo uranium ore deposits are the only known sites 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, as far as is currently known, to the Oklo ore bodies. It is
also possible that other natural nuclear fission reactors were once operating but have since been
geologically disturbed so much as to be unrecognizable, possibly even "diluting" the uranium so far
that the isotope ratio would no longer serve as a "fingerprint". Only a small part of the continental
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crust and no part of the oceanic crust reaches the age of the deposits at Oklo or an age during
which isotope ratios of natural uranium would have allowed a self-sustaining chain reaction with
water as a moderator.
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.[4]
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Uranium is naturally present in the rocks of the earth, and the abundance of fissile U was at
least 3% or higher at all times prior to reactor startup. Uranium is soluble in water only in the
presence of oxygen. Therefore, increasing oxygen levels during the aging of the 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 could not have taken
place.
It is estimated that nuclear reactions in the uranium in centimeter- to meter-sized veins consumed
235
about five tons of U and elevated temperatures to a few hundred degrees Celsius.[4][8] Most of
the non-volatile fission products and actinides have only moved centimeters in the veins during
the last 2 billion years.[4] Studies have suggested this as a useful natural analogue for nuclear
waste disposal.[9] The overall mass defect from the fission of five tons of 235U is about 4.6
kilograms (10 lb). Over its lifetime the reactor produced roughly 100 megatonnes of TNT (420 PJ)
in thermal energy, including neutrinos. If one ignores fission of plutonium (which makes up
roughly a third of fission events over the course of normal burnup in modern human-made light
water reactors), then fission product yields amount to roughly 129 kilograms (284 lb) of
technetium-99 (since decayed to ruthenium-99), 108 kilograms (238 lb) of zirconium-93 (since
decayed to niobium-93), 198 kilograms (437 lb) of caesium-135 (since decayed to barium-135, but
the real value is probably lower as its parent nuclide, xenon-135, is a strong neutron poison and
135
will have absorbed neutrons before decaying to Cs in some cases), 28 kilograms (62 lb) of
palladium-107 (since decayed to silver), 86 kilograms (190 lb) of strontium-90 (long since decayed
to zirconium), and 185 kilograms (408 lb) of caesium-137 (long since decayed to barium).
Relation to the atomic fine-structure constant
The natural reactor of Oklo has been used to check if the atomic fine-structure constant α might
have changed over the past 2 billion years. That is because α influences the rate of various nuclear
149 150
reactions. For example, Sm captures a neutron to become Sm, and since the rate of neutron
capture depends on the value of α, the ratio of the two samarium isotopes in samples from Oklo
can be used to calculate the value of α from 2 billion years ago.
Several studies have analysed the relative concentrations of radioactive isotopes left behind at
Oklo, and most have concluded that nuclear reactions then were much the same as they are today,
which implies that α was the same too.[10][11][12]
See also
Deep geological repository
Geology of Gabon
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Mounana
References
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External links
The natural nuclear reactor at Oklo: A comparison with modern nuclear reactors, Radiation
Information Network, April 2005 ([Link]
[Link]/radinf/Files/[Link])
Oklo Fossil Reactors ([Link]
search/oklo/[Link])
NASA Astronomy Picture of the Day: NASA, Oklo, Fossile Reactor, Zone 15 (16 October 2002)
([Link]
( הכור הגרעיני של הטבע[Link] (in Hebrew
language)
Retrieved from "[Link]
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