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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 have occurred in the past, are established by analysis of isotope ratios of uranium and of the fission products (and the stable daughter nuclides of those fission products). The first such fossil reactor was first discovered 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 noticed sharp depletions of fissionable 235
U
in gaseous uranium 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]
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 the 235
U
isotope. Where the usual concentrations of 235
U
were 0.72% the Oklo samples showed only 0.60%. This was a significant difference—the samples bore 17% less 235
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.
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 ore with a 235
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 234
U did not deviate significantly in its concentration from other natural samples. Both depleted uranium and reprocessed uranium will usually have 234
U concentrations significantly different from the secular equilibrium of 55 ppm 234
U relative to 238
U. This is due to 234
U being enriched together with 235
U and due to it being both consumed by neutron capture and produced from 235
U by fast neutron induced (n,2n) reactions in nuclear reactors. In Oklo any possible deviation of 234
U concentration present at the time the reactor was active would have long since decayed away. 236
U 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 thus basically nothing and below any abilities of current equipment to detect.
This loss in 235
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 |
The neodymium found at Oklo has a different isotopic composition to that of natural neodymium: the latter contains 27% 142
Nd
, while that of Oklo contains less than 6%. The 142
Nd
is not produced by fission; the ore contains both fission-produced and natural neodymium. From this 142
Nd
content, we can subtract the natural neodymium and gain access to the isotopic composition of neodymium produced by the fission of 235
U
. The two isotopes 143
Nd
and 145
Nd
lead to the formation of 144
Nd
and 146
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.
Similar investigations into the isotopic ratios of ruthenium at Oklo found a much higher 99
Ru
concentration than otherwise naturally occurring (27–30% vs. 12.7%). This anomaly could be explained by the decay of 99
Tc
to 99
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 235
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 subsequently beta decay and 100
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 100
Mo. On the timescale of when the reactors were in operation, very little (about 0.17 ppb) decay to 100
Ru
will have occurred. Other pathways of 100
Ru production like neutron capture in 99
Ru or 99
Tc (quickly followed by beta decay) can only have occurred during high neutron flux and thus ceased when the fission chain reaction stopped.
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.
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.
A key factor that made the reaction possible was that, at the time the reactor went critical 1.7 billion years ago, the fissile isotope 235
U
made up about 3.1% of the natural uranium, which is comparable to the amount used in some of today's reactors. (The remaining 96.9% was 238
U
and roughly 55 ppm 234
U, neither of which is fissile by slow or moderated neutrons.) Because 235
U
has a shorter half-life than 238
U
, and thus decays more rapidly, the current abundance of 235
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 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] Uranium is naturally present in the rocks of the earth, and the abundance of fissile 235
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.[ citation needed ] 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 about five tons of 235
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 235
U 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 will have absorbed neutrons before decaying to 135
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).
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 reactions. For example, 149
Sm
captures a neutron to become 150
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]
Nuclear fission is a reaction in which the nucleus of an atom splits into two or more smaller nuclei. The fission process often produces gamma photons, and releases a very large amount of energy even by the energetic standards of radioactive decay.
In nuclear physics, a nuclear chain reaction occurs when one single nuclear reaction causes an average of one or more subsequent nuclear reactions, thus leading to the possibility of a self-propagating series or "positive feedback loop" of these reactions. The specific nuclear reaction may be the fission of heavy isotopes. A nuclear chain reaction releases several million times more energy per reaction than any chemical reaction.
A nuclear reactor is a device used to initiate and control a fission nuclear chain reaction. Nuclear reactors are used at nuclear power plants for electricity generation and in nuclear marine propulsion. When a fissile nucleus like uranium-235 or plutonium-239 absorbs a neutron, it splits into lighter nuclei, releasing energy, gamma radiation, and free neutrons, which can induce further fission in a self-sustaining chain reaction. The process is carefully controlled using control rods and neutron moderators to regulate the number of neutrons that continue the reaction, ensuring the reactor operates safely, although inherent control by means of delayed neutrons also plays an important role in reactor output control. The efficiency of nuclear fuel is much higher than fossil fuels; the 5% enriched uranium used in the newest reactors has an energy density 120,000 times higher than coal.
Uranium is a chemical element with the symbol U and atomic number 92. It is a silvery-grey metal in the actinide series of the periodic table. A uranium atom has 92 protons and 92 electrons, of which 6 are valence electrons. Uranium radioactively decays, usually by emitting an alpha particle. The half-life of this decay varies between 159,200 and 4.5 billion years for different isotopes, making them useful for dating the age of the Earth. The most common isotopes in natural uranium are uranium-238 and uranium-235. Uranium has the highest atomic weight of the primordially occurring elements. Its density is about 70% higher than that of lead and slightly lower than that of gold or tungsten. It occurs naturally in low concentrations of a few parts per million in soil, rock and water, and is commercially extracted from uranium-bearing minerals such as uraninite.
In nuclear engineering, fissile material is material that can undergo nuclear fission when struck by a neutron of low energy. A self-sustaining thermal chain reaction can only be achieved with fissile material. The predominant neutron energy in a system may be typified by either slow neutrons or fast neutrons. Fissile material can be used to fuel thermal-neutron reactors, fast-neutron reactors and nuclear explosives.
The nuclear fuel cycle, also called nuclear fuel chain, is the progression of nuclear fuel through a series of differing stages. It consists of steps in the front end, which are the preparation of the fuel, steps in the service period in which the fuel is used during reactor operation, and steps in the back end, which are necessary to safely manage, contain, and either reprocess or dispose of spent nuclear fuel. If spent fuel is not reprocessed, the fuel cycle is referred to as an open fuel cycle ; if the spent fuel is reprocessed, it is referred to as a closed fuel cycle.
Uranium-238 is the most common isotope of uranium found in nature, with a relative abundance of 99%. Unlike uranium-235, it is non-fissile, which means it cannot sustain a chain reaction in a thermal-neutron reactor. However, it is fissionable by fast neutrons, and is fertile, meaning it can be transmuted to fissile plutonium-239. 238U cannot support a chain reaction because inelastic scattering reduces neutron energy below the range where fast fission of one or more next-generation nuclei is probable. Doppler broadening of 238U's neutron absorption resonances, increasing absorption as fuel temperature increases, is also an essential negative feedback mechanism for reactor control.
Nuclear fission products are the atomic fragments left after a large atomic nucleus undergoes nuclear fission. Typically, a large nucleus like that of uranium fissions by splitting into two smaller nuclei, along with a few neutrons, the release of heat energy, and gamma rays. The two smaller nuclei are the fission products..
Uranium-234 is an isotope of uranium. In natural uranium and in uranium ore, 234U occurs as an indirect decay product of uranium-238, but it makes up only 0.0055% of the raw uranium because its half-life of just 245,500 years is only about 1/18,000 as long as that of 238U. Thus the ratio of 234
U to 238
U in a natural sample is equivalent to the ratio of their half-lives. The primary path of production of 234U via nuclear decay is as follows: uranium-238 nuclei emit an alpha particle to become thorium-234. Next, with a short half-life, 234Th nuclei emit a beta particle to become protactinium-234 (234Pa), or more likely a nuclear isomer denoted 234mPa. Finally, 234Pa or 234mPa nuclei emit another beta particle to become 234U nuclei.
Uranium (92U) is a naturally occurring radioactive element (radioelement) with no stable isotopes. It has two primordial isotopes, uranium-238 and uranium-235, that have long half-lives and are found in appreciable quantity in Earth's crust. The decay product uranium-234 is also found. Other isotopes such as uranium-233 have been produced in breeder reactors. In addition to isotopes found in nature or nuclear reactors, many isotopes with far shorter half-lives have been produced, ranging from 214U to 242U. The standard atomic weight of natural uranium is 238.02891(3).
Naturally occurring neodymium (60Nd) is composed of five stable isotopes, 142Nd, 143Nd, 145Nd, 146Nd and 148Nd, with 142Nd being the most abundant (27.2% natural abundance), and two long-lived radioisotopes, 144Nd and 150Nd. In all, 35 radioisotopes of neodymium have been characterized up to now, with the most stable being naturally occurring isotopes 144Nd (alpha decay, a half-life (t1/2) of 2.29×1015 years) and 150Nd (double beta decay, t1/2 of 9.3×1018 years), and for practical purposes they can be considered to be stable as well. All of the remaining radioactive isotopes have half-lives that are less than 12 days, and the majority of these have half-lives that are less than 70 seconds; the most stable artificial isotope is 147Nd with a half-life of 10.98 days. This element also has 15 known meta states with the most stable being 139mNd (t1/2 5.5 hours), 135mNd (t1/2 5.5 minutes) and 133m1Nd (t1/2 ~70 seconds).
Nuclear reactor physics is the field of physics that studies and deals with the applied study and engineering applications of chain reaction to induce a controlled rate of fission in a nuclear reactor for the production of energy.
The thorium fuel cycle is a nuclear fuel cycle that uses an isotope of thorium, 232
Th
, as the fertile material. In the reactor, 232
Th
is transmuted into the fissile artificial uranium isotope 233
U
which is the nuclear fuel. Unlike natural uranium, natural thorium contains only trace amounts of fissile material, which are insufficient to initiate a nuclear chain reaction. Additional fissile material or another neutron source is necessary to initiate the fuel cycle. In a thorium-fuelled reactor, 232
Th
absorbs neutrons to produce 233
U
. This parallels the process in uranium breeder reactors whereby fertile 238
U
absorbs neutrons to form fissile 239
Pu
. Depending on the design of the reactor and fuel cycle, the generated 233
U
either fissions in situ or is chemically separated from the used nuclear fuel and formed into new nuclear fuel.
Spent nuclear fuel, occasionally called used nuclear fuel, is nuclear fuel that has been irradiated in a nuclear reactor. It is no longer useful in sustaining a nuclear reaction in an ordinary thermal reactor and, depending on its point along the nuclear fuel cycle, it will have different isotopic constituents than when it started.
This page discusses each of the main elements in the mixture of fission products produced by nuclear fission of the common nuclear fuels uranium and plutonium. The isotopes are listed by element, in order by atomic number.
Xenon-135 (135Xe) is an unstable isotope of xenon with a half-life of about 9.2 hours. 135Xe is a fission product of uranium and it is the most powerful known neutron-absorbing nuclear poison, with a significant effect on nuclear reactor operation. The ultimate yield of xenon-135 from fission is 6.3%, though most of this is from fission-produced tellurium-135 and iodine-135.
Uranium-236 is an isotope of uranium that is neither fissile with thermal neutrons, nor very good fertile material, but is generally considered a nuisance and long-lived radioactive waste. It is found in spent nuclear fuel and in the reprocessed uranium made from spent nuclear fuel.
Long-lived fission products (LLFPs) are radioactive materials with a long half-life produced by nuclear fission of uranium and plutonium. Because of their persistent radiotoxicity, it is necessary to isolate them from humans and the biosphere and to confine them in nuclear waste repositories for geological periods of time. The focus of this article is radioisotopes (radionuclides) generated by fission reactors.
The liquid fluoride thorium reactor is a type of molten salt reactor. LFTRs use the thorium fuel cycle with a fluoride-based molten (liquid) salt for fuel. In a typical design, the liquid is pumped between a critical core and an external heat exchanger where the heat is transferred to a nonradioactive secondary salt. The secondary salt then transfers its heat to a steam turbine or closed-cycle gas turbine.
Nuclear transmutation is the conversion of one chemical element or an isotope into another chemical element. Nuclear transmutation occurs in any process where the number of protons or neutrons in the nucleus of an atom is changed.