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Tuesday, May 29, 2018

Liquid fluoride thorium reactor

From Wikipedia, the free encyclopedia

Liquid FLiBe salt

The liquid fluoride thorium reactor (acronym LFTR; often pronounced lifter) 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.[1]

Molten-salt-fueled reactors (MSRs) supply the nuclear fuel mixed into a molten salt. They should not be confused with designs that use a molten salt for cooling only (fluoride high-temperature reactors, FHRs) and still have a solid fuel.[2] Molten salt reactors, as a class, include both burners and breeders in fast or thermal spectra, using fluoride or chloride salt-based fuels and a range of fissile or fertile consumables. LFTRs are defined by the use of fluoride fuel salts and the breeding of thorium into uranium-233 in the thermal spectrum.

The LFTR concept was first investigated at the Oak Ridge National Laboratory Molten-Salt Reactor Experiment in the 1960s, though the MSRE did not use thorium. The LFTR has recently been the subject of a renewed interest worldwide.[3] Japan, China, the UK and private US, Czech, Canadian[4] and Australian companies have expressed the intent to develop, and commercialize the technology.

LFTRs differ from other power reactors in almost every aspect: they use thorium that is turned into uranium, instead of using uranium directly; they are refueled by pumping without shutdown; they use a liquid salt coolant, which allows for higher operating temperatures, and which thereby allows for much lower pressure in the system.[5] These distinctive characteristics give rise to many potential advantages, as well as design challenges.

Background

Tiny crystals of thorite, a thorium mineral, under magnification.
 
Molten salt reactor at Oak Ridge

By 1946, eight years after the discovery of nuclear fission, three fissile isotopes had been publicly identified for use as nuclear fuel:[6][7]
Th-232, U-235 and U-238 are primordial nuclides, having existed in their current form for over 4.5 billion years, predating the formation of the Earth; they were forged in the cores of dying stars through the r-process and scattered across the galaxy by supernovas.[9] Their radioactive decay produces about half of the earth's internal heat.[10]

For technical and historical[11] reasons, the three are each associated with different reactor types. U-235 is the world's primary nuclear fuel and is usually used in light water reactors. U-238/Pu-239 has found the most use in liquid sodium fast breeder reactors and CANDU Reactors. Th-232/U-233 is best suited to molten salt reactors (MSR).[12]

Alvin M. Weinberg pioneered the use of the MSR at Oak Ridge National Laboratory. At ORNL, two prototype molten salt reactors were successfully designed, constructed and operated. These were the Aircraft Reactor Experiment in 1954 and Molten-Salt Reactor Experiment from 1965 to 1969. Both test reactors used liquid fluoride fuel salts. The MSRE notably demonstrated fueling with U-233 and U-235 during separate test runs.[13](pix) Weinberg was removed from his post and the MSR program closed down in the early 1970s,[14] after which research stagnated in the United States.[15][16] Today, the ARE and the MSRE remain the only molten salt reactors ever operated.

Breeding basics

In a nuclear power reactor, there are two types of fuel. The first is fissile material, which splits when hit by neutrons, releasing a large amount of energy and also releasing two or three new neutrons. These can split more fissile material, resulting in a continued chain reaction. Examples of fissile fuels are U-233, U-235 and Pu-239. The second type of fuel is called fertile. Examples of fertile fuel are Th-232 (mined thorium) and U-238 (mined uranium). Often the amount of fertile fuel in the reactor is far greater than the amount of fissile, but it cannot be fissioned directly. It must first absorb one of the 2 or 3 neutrons produced in the fission process, which is called neutron capture, then it becomes a fissile isotope by radioactive decay. This process is called breeding.[5]

All reactors breed some fuel this way,[17] but today's solid fueled thermal reactors don't breed enough new fuel from the fertile to make up for the amount of fissile they consume. This is because today's reactors use the mined uranium-plutonium cycle in a moderated neutron spectrum. Such a fuel cycle, using slowed down neutrons, gives back less than 2 new neutrons from fissioning the bred plutonium. Since 1 neutron is required to sustain the fission reaction, this leaves a budget of less than 1 neutron per fission to breed new fuel. In addition, the materials in the core such as metals, moderators and fission products absorb some neutrons, leaving too few neutrons to breed enough fuel to continue operating the reactor. As a consequence they must add new fissile fuel periodically and swap out some of the old fuel to make room for the new fuel.

In a reactor that breeds at least as much new fuel as it consumes, it is not necessary to add new fissile fuel. Only new fertile fuel is added, which breeds to fissile inside the reactor. In addition the fission products need to be removed. This type of reactor is called a breeder reactor. If it breeds just as much new fissile from fertile to keep operating indefinitely, it is called a break-even breeder or isobreeder. A LFTR is usually designed as a breeder reactor: thorium goes in, fission products come out.

Reactors that use the uranium-plutonium fuel cycle require fast reactors to sustain breeding, because only with fast moving neutrons does the fission process provide more than 2 neutrons per fission. With thorium, it is possible to breed using a thermal reactor. This was proven to work in the Shippingport Atomic Power Station, whose final fuel load bred slightly more fissile from thorium than it consumed, despite being a fairly standard light water reactor. Thermal reactors require less of the expensive fissile fuel to start, but are more sensitive to fission products left in the core.

There are two ways to configure a breeder reactor to do the required breeding. One can place the fertile and fissile fuel together, so breeding and splitting occurs in the same place. Alternatively, fissile and fertile can be separated. The latter is known as core-and-blanket, because a fissile core produces the heat and neutrons while a separate blanket does all the breeding.

Reactor primary system design variations

Oak Ridge investigated both ways to make a breeder for their molten salt breeder reactor. Because the fuel is liquid, they are called the "single fluid" and "two fluid" thorium thermal breeder molten salt reactors.

Single fluid reactor

Simplified schematic of a single fluid reactor.

The one-fluid design includes a large reactor vessel filled with fluoride salt containing thorium and uranium. Graphite rods immersed in the salt function as a moderator and to guide the flow of salt. In the ORNL MSBR design[18] a reduced amount of graphite near the edge of the reactor core would make the outer region under-moderated, and increased the capture of neutrons there by the thorium. With this arrangement, most of the neutrons were generated at some distance from the reactor boundary, and reduced the neutron leakage to an acceptable level.[19] Still, a single fluid design needs a considerable size to permit breeding.[20]

In a breeder configuration, extensive fuel processing was specified to remove fission products from the fuel salt.[13](p181) In a converter configuration fuel processing requirement was simplified to reduce plant cost.[19] The trade-off was the requirement of periodic uranium refueling.

The MSRE was a core region only prototype reactor.[21] The MSRE provided valuable long-term operating experience. According to estimates of Japanese scientists, a single fluid LFTR program could be achieved through a relatively modest investment of roughly 300-400 million dollars over 5–10 years to fund research to fill minor technical gaps and build a small reactor prototype comparable to the MSRE.[22]

Two fluid reactor

The two-fluid design is mechanically more complicated compared to the "single fluid" reactor design. The "two fluid" reactor has a high-neutron-density core that burns uranium-233 from the thorium fuel cycle. A separate blanket of thorium salt absorbs the neutrons and its thorium is converted to protactinium-233. Protactinium-233 can be left in the blanket region where neutron flux is lower, so that it slowly decays to U-233 fissile fuel,[23] rather than capture neutrons. This bred fissile U-233 can be recovered by simple fluorination, and placed in the core to fission. The core's salt is also purified, first by fluorination to remove uranium, then vacuum distillation to remove and reuse the carrier salts. The still bottoms left after the distillation are the fission products waste of a LFTR.

The advantages of separating the core and blanket fluid include:
  1. Simplified fuel processing. Thorium is chemically similar to several fission products, called lanthanides. With thorium in a separate blanket, thorium is kept isolated from the lanthanides. Without thorium in the core fluid, removal of lanthanide fission products is simplified.
  2. Low fissile inventory. Because the fissile fuel is concentrated in a small core fluid, the actual reactor core is more compact. There is no fissile material in the outer blanket that contains the fertile fuel for breeding. Because of this, the 1968 ORNL design required just 315 kilograms of fissile materials to start up a 250 MW(e) two fluid MSBR reactor.[24](p35) This reduces the cost of the initial fissile startup charge, and allows more reactors to be started up on any given amount of fissile material.
  3. More efficient breeding. The thorium blanket can effectively capture leaked neutrons from the core region. There is nearly zero fission occurring in the blanket, so the blanket itself does not leak significant numbers of neutrons. This results in a high efficiency of neutron use (neutron economy), and a higher breeding ratio, especially with small reactors.
One design weakness of the two-fluid design is the necessity for a barrier wall between the core and the blanket region, a wall that would have to be replaced periodically because of fast neutron damage.[25](p29) Graphite was the material chosen by ORNL because of its low neutron absorption, compatibility with the molten salts, high temperature resistance, and sufficient strength and integrity to separate the fuel and blanket salts. The effect of neutron radiation on graphite is to slowly shrink and then swell the graphite to cause an increase in porosity and a deterioration in physical properties.[24](p13) Graphite pipes would change length, and may crack and leak. ORNL chose not to pursue the two-fluid design, and no examples of the two-fluid reactor were ever constructed.

One additional design weakness of the two-fluid design was its complex plumbing. ORNL thought it necessary to use complex interleaving of the core and blanket piping in order to get a high reactor power level with acceptably low power density.[24](p4) More recent research has put into question the need for complex interleaving graphite tubing, suggesting a simple elongated tube-in-shell reactor would allow high total reactor power without complex tubing.[1](p6)

Hybrid "one and a half fluid" reactor

A two fluid reactor that has thorium in the fuel salt is sometimes called a "one and a half fluid" reactor, or 1.5 fluid reactor.[26] This is a hybrid, with some of the advantages and disadvantages of both 1 fluid and 2 fluid reactors. Like the 1 fluid reactor, it has thorium in the fuel salt, which complicates the fuel processing. And yet, like the 2 fluid reactor, it can use a highly effective separate blanket to absorb neutrons that leak from the core. The added disadvantage of keeping the fluids separate using a barrier remains, but with thorium present in the fuel salt there are fewer neutrons that must pass through this barrier into the blanket fluid. This results in less damage to the barrier. Any leak in the barrier would also be of lower consequence, as the processing system must already deal with thorium in the core.

The main design question when deciding between a one and a half or two fluid LFTR is whether a more complicated reprocessing or a more demanding structural barrier will be easier to solve.

Calculated nuclear performance of 1000-MW(e) MSBR design concepts[25](p29)
Design concept Breeding ratio Fissile inventory
Single-fluid, 30 year graphite life, fuel processing 1.06 2300 kg
Single-fluid, 4 year graphite life, fuel processing 1.06 1500 kg
1.5 fluid, replaceable core, fuel processing 1.07 900 kg
Two-fluid, replaceable core, fuel processing 1.07 700 kg

Power generation

The LFTR with a high operating temperature of 700 degrees Celsius can operate at a thermal efficiency to electrical of 45%.[23] This is higher than today's light water reactors (LWRs) that are at 32-36% thermal to electrical efficiency. In addition to electricity generation, concentrated thermal energy from LFTR can enable application as Industrial process heat for many uses, such as ammonia production with the Haber process or thermal Hydrogen production by water splitting.

Rankine cycle

Rankine steam cycle

The Rankine cycle is the most basic thermodynamic power cycle. The simplest cycle consists of a steam generator, a turbine, a condenser, and a pump. The working fluid is usually water. A Rankine power conversion system coupled to a LFTR could take advantage of increased steam temperature to improve its thermal efficiency.[27] The subcritical Rankine steam cycle is currently used in commercial power plants, with the newest plants utilizing the higher temperature, higher pressure, supercritical Rankine steam cycles. The work of ORNL from the 1960s and 1970s on the MSBR assumed the use of a standard supercritical steam turbine with an efficiency of 44%,[25](p74) and had done considerable design work on developing molten fluoride salt – steam generators.[28]

Brayton cycle


The working gas of a Brayton cycle can be helium, nitrogen, or carbon dioxide. The high-pressure working gas is expanded in a turbine to produce power. The low-pressure warm gas is cooled in an ambient cooler. The low-pressure cold gas is compressed to the high-pressure of the system. Often the turbine and the compressor are mechanically connected through a single shaft.[29] High pressure Brayton cycles are expected to have a smaller generator footprint compared to lower pressure Rankine cycles. A Brayton cycle heat engine can operate at lower pressure with wider diameter piping.[29] The world's first commercial Brayton cycle solar power module (100 kW) was built and demonstrated in Israel's Arava Desert in 2009.[30]

Removal of fission products

The LFTR needs a mechanism to remove the fission products from the fuel. Fission products left in the reactor absorb neutrons and thus reduce the production of new fissile fuel. This is especially important in the thorium fuel cycle with few spare neutrons and a thermal neutron spectrum, where absorption is strong. The minimum requirement is to recover the valuable fissile material from used fuel.

Removal of fission products is similar to reprocessing of solid fuel elements - by chemical or physical means the highly valuable fissile fuel is separated from the waste fission products. Ideally the fertile fuel (thorium or U-238) and other fuel components (e.g. carrier salt or fuel cladding in solid fuels) can also be reused for new fuel. However, for economic reasons they may also end up in the waste.

As the fuel of a LFTR is a molten salt mixture, it is attractive to use pyroprocessing, high temperature methods working directly from the hot molten salt. Pyroprocessing does not use radiation sensitive solvents and is not easily disturbed by decay heat. It can be used on the highly radioactive fuel directly from the reactor.[31] Having the chemical separation on site, close to the reactor avoids transport and keeps the total inventory of the fuel cycle low. Ideally everything except new fuel (thorium) and waste (fission products) stays inside the plant.

On site processing is planned to work continuously, cleaning a small fraction of the salt every day and sending it back to the reactor. There is no need to make the fuel salt very clean; the purpose is to keep the concentration of fission products and other impurities (e.g. oxygen) low enough. Especially the concentrations of some of the rare earth elements need to be kept low, as they have a large cross section for neutron capture. Some other elements with a small cross section like Cs or Zr may accumulate over years of operation before they are removed.

One potential advantage of having the fuel in liquid-phase is that it not only facilitates separating fission-products from the fuel, but also separating the fission products from each other, which is highly lucrative for certain isotopes that are scarce and in high-demand for various industrial (radiation sources for testing welds via radiography), agricultural (sterilizing produce via irradiation), and medical (Molybdenum-99 which decays into Technetium-99m which is a highly sought-after radiolabel dye for marking cancerous cells in medical-scans).

The more noble metals (Pd, Ru, Ag, Mo, Nb, Sb, Tc) do not form fluorides in the normal salt, but form fine metallic particles in the salt. They can plate out at metal surfaces like the heat exchanger or some kinds of high surface area filters that are easier to remove. Still there is some uncertainty where these noble elements end up, as the MSRE only provided a relatively short operating experience and independent laboratory experiments are difficult.[32]

Some elements like Xe and Kr come out easily as gas, assisted by a sparge of helium. In addition a part of the "noble" metals are removed together with the gas as a fine mist. Especially the fast removal of Xe-135 is important, as this is a very strong neutron poison and makes reactor control more difficult if left in the reactor. Removal of Xe also improves neutron economy. The gas (mainly He, Xe and Kr) is held up for about 2 days until a large fraction of the Xe-135 and other short lived isotopes have decayed. Most of the gas can then be recycled. After an additional hold up of several months, radioactivity is low enough to separate the gas at low temperatures into helium (for reuse), xenon (for sale) and krypton. The krypton needs storage (e.g. in compressed form) for an extended time (several decades) to wait for the decay of Kr-85.[18](p274)

For cleaning the salt mixture several methods of chemical separation were proposed.[33] Compared to classical PUREX reprocessing, pyroprocessing can be more compact and produce less secondary waste. The pyroprocesses of the LFTR salt already starts with a suitable liquid form, so it may be less expensive than using solid oxide fuels. However, because no complete molten salt reprocessing plant has been built, all testing has been limited to the laboratory, and with only a few elements. There is still more research and development needed to improve separation and make reprocessing more economically viable.

Uranium and some other elements can be removed from the salt by a process called fluorine volatility: A sparge of fluorine removes volatile high-valence fluorides as a gas. This is mainly uranium hexafluoride, containing the uranium-233 fuel, but also neptunium hexafluoride, technetium hexafluoride and selenium hexafluoride, as well as fluorides of some other fission products (e.g. iodine, molybdenum and tellurium). The volatile fluorides can be further separated by adsorption and distillation. Handling uranium hexafluoride is well established in enrichment. The higher valence fluorides are quite corrosive at high temperatures and require more resistant materials than Hastelloy. One suggestion in the MSBR program at ORNL was using solidified salt as a protective layer. At the MSRE reactor fluorine volatility was used to remove uranium from the fuel salt. Also for use with solid fuel elements fluorine volatility is quite well developed and tested.[31]

Another simple method, tested during the MSRE program, is high temperature vacuum distillation. The lower boiling point fluorides like uranium tetrafluoride and the LiF and BeF carrier salt can be removed by distillation. Under vacuum the temperature can be lower than the ambient pressure boiling point. So a temperature of about 1000 °C is sufficient to recover most of the FLiBe carrier salt.[34] However, while possible in principle, separation of thorium fluoride from the even higher boiling point lanthanide fluorides would require very high temperatures and new materials. The chemical separation for the 2-fluid designs, using uranium as a fissile fuel can work with these two relatively simple processes:[35] Uranium from the blanket salt can be removed by fluorine volatility, and transferred to the core salt. To remove the fissile products from the core salt, first the uranium is removed via fluorine volatility. Then the carrier salt can be recovered by high temperature distillation. The fluorides with a high boiling point, including the lanthanides stay behind as waste.

The early Oak Ridge's chemistry designs were not concerned with proliferation and aimed for fast breeding. They planned to separate and store protactinium-233, so it could decay to uranium-233 without being destroyed by neutron capture in the reactor. With a half-life of 27 days, 2 months of storage would assure that 75% of the 233Pa decays to 233U fuel. The protactinium removal step is not required per se for a LFTR. Alternate solutions are operating at a lower power density and thus a larger fissile inventory (for 1 or 1.5 fluid) or a larger blanket (for 2 fluid). Also a harder neutron spectrum helps to achieve acceptable breeding without protactinium isolation.[1]

If Pa separation is specified, this must be done quite often (for example, every 10 days) to be effective. For a 1 GW, 1-fluid plant this means about 10% of the fuel or about 15 t of fuel salt need to go through reprocessing every day. This is only feasible if the costs are much lower than current costs for reprocessing solid fuel.

Newer designs usually avoid the Pa removal[1] and send less salt to reprocessing, which reduces the required size and costs for the chemical separation. It also avoids proliferation concerns due to high purity U-233 that might be available from the decay of the chemical separated Pa.

Separation is more difficult if the fission products are mixed with thorium, because thorium, plutonium and the lanthanides (rare earth elements) are chemically similar. One process suggested for both separation of protactinium and the removal of the lanthanides is the contact with molten bismuth. In a redox-reaction some metals can be transferred to the bismuth melt in exchange for lithium added to the bismuth melt. At low lithium concentrations U, Pu and Pa move to the bismuth melt. At more reducing conditions (more lithium in the bismuth melt) the lanthanides and thorium transfer to the bismuth melt too. The fission products are then removed from the bismuth alloy in a separate step, e.g. by contact to a LiCl melt.[36] However this method is far less developed. A similar method may also be possible with other liquid metals like aluminum.[37]

Advantages

Thorium-fueled molten salt reactors offer many potential advantages compared to conventional solid uranium fueled light water reactors:[8][20][38][39][40][41]

Safety

  • Inherent safety. LFTR designs use a strong negative temperature coefficient of reactivity to achieve passive inherent safety against excursions of reactivity. The temperature dependence comes from 3 sources. The first is that thorium absorbs more neutrons if it overheats, the so-called Doppler effect.[42] This leaves fewer neutrons to continue the chain reaction, reducing power. The second part is heating the graphite moderator, that usually causes a positive contribution to the temperature coefficient.[42] The third effect has to do with thermal expansion of the fuel.[42] If the fuel overheats, it expands considerably, which, due to the liquid nature of the fuel, will push fuel out of the active core region. In a small (e.g. the MSRE test reactor) or well moderated core this reduces the reactivity. However, in a large, under-moderated core (e.g. the ORNL MSBR design), less fuel salt means better moderation and thus more reactivity and an undesirable positive temperature coefficient.
  • Stable coolant. Molten fluorides are chemically stable and impervious to radiation. The salts do not burn, explode, or decompose, even under high temperature and radiation.[43] There are no rapid violent reactions with water and air that sodium coolant has. There is no combustible hydrogen production that water coolants have.[44] However the salt is not stable to radiation at low (less than 100 C) temperatures due to radiolysis.
  • Low pressure operation. Because the coolant salts remain liquid at high temperatures,[43] LFTR cores are designed to operate at low pressures, like 0.6 MPa[45] (comparable to the pressure in the drinking water system) from the pump and hydrostatic pressure. Even if the core fails[clarification needed], there is little increase in volume. Thus the containment building cannot blow up. LFTR coolant salts are chosen to have very high boiling points. Even a several hundred degree heatup during a transient or accident does not cause a meaningful pressure increase. There is no water or hydrogen in the reactor that can cause a large pressure rise or explosion as happened during the Fukushima Daiichi nuclear accident.[46][unreliable source]
  • No pressure buildup from fission. LFTRs are not subject to pressure buildup of gaseous and volatile fission products. The liquid fuel allows for online removal of gaseous fission products, such as xenon, for processing, thus these decay products would not be spread in a disaster.[47] Further, fission products are chemically bonded to the fluoride-salt, including iodine,[dubious ] cesium, and strontium, capturing the radiation and preventing the spread of radioactive material to the environment.[48]
  • Easier to control. A molten fuel reactor has the advantage of easy removal of xenon-135. Xenon-135, an important neutron absorber, makes solid fueled reactors difficult to control. In a molten fueled reactor, xenon-135 can be removed. In solid-fuel reactors, xenon-135 remains in the fuel and interferes with reactor control.[49]
  • Slow heatup. Coolant and fuel are inseparable, so any leak or movement of fuel will be intrinsically accompanied by a large amount of coolant. Molten fluorides have high volumetric heat capacity, some such as FLiBe, even higher than water. This allows them to absorb large amounts of heat during transients or accidents.[33][50]
  • Passive decay heat cooling. Many reactor designs (such as that of the Molten-Salt Reactor Experiment) allow the fuel/coolant mixture to escape to a drain tank, when the reactor is not running (see "Fail safe core" below). This tank is planned to have some kind (details are still open) of passive decay heat removal, thus relying on physical properties (rather than controls) to operate.[51]
  • Fail safe core. LFTRs can include a freeze plug at the bottom that has to be actively cooled, usually by a small electric fan. If the cooling fails, say because of a power failure, the fan stops, the plug melts, and the fuel drains to a subcritical passively cooled storage facility. This not only stops the reactor, also the storage tank can more easily shed the decay heat from the short-lived radioactive decay of irradiated nuclear fuels. Even in the event of a major leak from the core such as a pipe breaking, the salt will spill onto the kitchen-sink-shaped room the reactor is in, which will drain the fuel salt by gravity into the passively cooled dump tank.[19]
  • Less long-lived waste. LFTRs can dramatically reduce the long-term radiotoxicity of their reactor wastes. Light water reactors with uranium fuel have fuel that is more than 95% U-238. These reactors normally transmute part of the U-238 to Pu-239, a long-lived isotope. Almost all of the fuel is therefore only one step away from becoming a transuranic long-lived element. Plutonium-239 has a half life of 24,000 years, and is the most common transuranic in spent nuclear fuel from light water reactors. Transuranics like Pu-239 cause the perception that reactor wastes are an eternal problem. In contrast, the LFTR uses the thorium fuel cycle, which transmutes thorium to U-233. Because thorium is a lighter element, more neutron captures are required to produce the transuranic elements. U-233 has two chances to fission in a LFTR. First as U-233 (90% will fission) and then the remaining 10% has another chance as it transmutes to U-235 (80% will fission). The fraction of fuel reaching neptunium-237, the most likely transuranic element, is therefore only 2%, about 15 kg per GWe-year.[52] This is a transuranic production 20x smaller than light water reactors, which produce 300 kg of transuranics per GWe-year. Importantly, because of this much smaller transuranic production, it is much easier to recycle the transuranics. That is, they are sent back to the core to eventually fission. Reactors operating on the U238-plutonium fuel cycle produce far more transuranics, making full recycle difficult on both reactor neutronics and the recycling system. In the LFTR, only a fraction of a percent, as reprocessing losses, goes to the final waste. When these two benefits of lower transuranic production, and recycling, are combined, a thorium fuel cycle reduces the production of transuranic wastes by more than a thousand-fold compared to a conventional once-through uranium-fueled light water reactor. The only significant long-lived waste is the uranium fuel itself, but this can be used indefinitely by recycling, always generating electricity.

    If the thorium stage ever has to be shut down, part of the reactors can be shut down and their uranium fuel inventory burned out in the remaining reactors, allowing a burndown of even this final waste to as small a level as society demands.[53] The LFTR does still produce radioactive fission products in its waste, but they don't last very long - the radiotoxicity of these fission products is dominated by cesium-137 and strontium-90. The longer half-life is cesium: 30.17 years. So, after 30.17 years, decay reduces the radioactivity by a half. Ten half-lives will reduce the radioactivity by two raised to a power of ten, a factor of 1,024. Fission products at that point, in about 300 years, are less radioactive than natural uranium.[54][55] What's more, the liquid state of the fuel material allows separation of the fission products not only from the fuel, but from each other as well, which enables them to be sorted by the length of each fission product's half-life, so that the ones with shorter half-lives can be brought out of storage sooner than those with longer half-lives.
  • Proliferation resistance. In 2016, Nobel Laureate physicist Dr Carlo Rubbia, former Director General of CERN, claimed a primary reason for the United States cutting thorium reactor research in the 1970s is what makes it so attractive today: thorium is difficult to turn into a nuclear weapon.[56][unreliable source?]

    The LFTR resists diversion of its fuel to nuclear weapons in four ways: first, the thorium-232 breeds by converting first to protactinium-233, which then decays to uranium-233. If the protactinium remains in the reactor, small amounts of U-232 are also produced. U-232 has a decay chain product (thallium-208) that emits powerful, dangerous gamma rays. These are not a problem inside a reactor, but in a bomb, they complicate bomb manufacture, harm electronics and reveal the bomb's location.[57] The second proliferation resistant feature comes from the fact that LFTRs produce very little plutonium, around 15 kg per gigawatt-year of electricity (this is the output of a single large reactor over a year). This plutonium is also mostly Pu-238, which makes it unsuitable for fission bomb building, due to the high heat and spontaneous neutrons emitted. The third track, a LFTR doesn't make much spare fuel. It produces at most 9% more fuel than it burns each year, and it's even easier to design a reactor that makes only 1% more fuel. With this kind of reactor, building bombs quickly will take power plants out of operation, and this is an easy indication of national intentions. And finally, use of thorium can reduce and eventually eliminate the need to enrich uranium. Uranium enrichment is one of the two primary methods by which states have obtained bomb making materials.[8]

Economy and efficiency

Comparison of annual fuel requirements and waste products of a 1 GW uranium-fueled LWR and 1 GW thorium-fueled LFTR power plant.[58]
  • Thorium abundance. A LFTR breeds thorium into uranium-233 fuel. The Earth's crust contains about three to four times as much thorium as U-238 (thorium is about as abundant as lead). It is a byproduct of rare-earth mining, normally discarded as waste. Using LFTRs, there is enough affordable thorium to satisfy the global energy needs for hundreds of thousands of years.[59] Thorium is more common in the earth’s crust than tin, mercury, or silver.[8] A cubic meter of average crust yields the equivalent of about four sugar cubes of thorium, enough to supply the energy needs of one person for more than ten years if completely fissioned.[8] Lemhi Pass on the Montana-Idaho border is estimated to contain 1,800,000 tons of high-grade thorium ore.[8] Five hundred tons could supply all U.S. energy needs for one year.[8] Due to lack of current demand, the U.S. government has returned about 3,200 metric tons of refined thorium nitrate to the crust, burying it in the Nevada desert.[8]
  • No shortage of natural resources. Sufficient other natural resources such as beryllium, lithium, nickel and molybdenum are available to build thousands of LFTRs.[60]
  • Reactor efficiency. Conventional reactors consume less than one percent of the mined uranium, leaving the rest as waste. With perfectly working reprocessing LFTR may consume up to about 99% of its thorium fuel. The improved fuel efficiency means that 1 ton of natural thorium in a LFTR produces as much energy as 35 t of enriched uranium in conventional reactors (requiring 250 t of natural uranium),[8] or 4,166,000 tons of black coal in a coal power plant.
  • Thermodynamic efficiency. LFTRs operating with modern supercritical steam turbines would operate at 45% thermal to electrical efficiency. With future closed gas Brayton cycles, which could be used in a LFTR power plant due to its high temperature operation, the efficiency could be up to 54%. This is 20 to 40% higher than today's light water reactors (33%), resulting in the same 20 to 40% reduction in fissile and fertile fuel consumption, fission products produced, waste heat rejection for cooling, and reactor thermal power.[8]
  • No enrichment and fuel element fabrication. Since 100% of natural thorium can be used as a fuel, and the fuel is in the form of a molten salt instead of solid fuel rods, expensive fuel enrichment and solid fuel rods' validation procedures and fabricating processes are not needed. This greatly decreases LFTR fuel costs. Even if the LFTR is started up on enriched uranium, it only needs this enrichment once just to get started. After startup, no further enrichment is required.[8]
  • Lower fuel cost. The salts are fairly inexpensive compared to solid fuel production. For example, while beryllium is quite expensive per kg, the amount of beryllium required for a large 1 GWe reactor is quite small. ORNL's MSBR required 5.1 tons of beryllium metal, as 26 tons of BeF2.[60] At a price of $147/kg BeF2,[50](p44) this inventory would cost less than $4 million, a modest cost for a multibillion-dollar power plant. Consequently, a beryllium price increase over the level assumed here has little effect in the total cost of the power plant. The cost of enriched lithium-7 is less certain, at $120–800/kg LiF.[1] and an inventory (again based on the MSBR system) of 17.9 tons lithium-7 as 66.5 tons LiF[60] makes between $8 million and $53 million for the LiF. Adding the 99.1 tons of thorium at $30/kg adds only $3 million. Fissile material is more expensive, especially if expensively reprocessed plutonium is used, at a cost of $100 per gram fissile plutonium. With a startup fissile charge of only 1.5 tons, made possible through the soft neutron spectrum[1] this makes $150 million. Adding everything up brings the total cost of the one time fuel charge at $165 to $210 million. This is similar to the cost of a first core for a light water reactor.[61] Depending on the details of reprocessing the salt inventory once can last for decades, whereas the LWR needs a completely new core every 4 to 6 years (1/3 is replaced every 12 to 24 months). ORNL's own estimate for the total salt cost of even the more expensive 3 loop system was around $30 million, which is less than $100 million in today's money.[62]
  • LFTRs are cleaner: as a fully recycling system, the discharge wastes from a LFTR are predominantly fission products, most of which (83%) have relatively short half lives in hours or days[63] compared to longer-lived actinide wastes of conventional nuclear power plants.[57] This results in a significant reduction in the needed waste containment period in a geologic repository. The remaining 17% of waste products require only 300 years until reaching background levels.[63] The radiotoxicity of the thorium fuel cycle waste is about 10,000 times less than that of one through uranium fuel.[8]
  • Less fissile fuel needed. Because LFTRs are thermal spectrum reactors, they need much less fissile fuel to get started. Only 1-2 tons of fissile are required to start up a single fluid LFTR, and potentially as low as 0.4 ton for a two fluid design.[1] In comparison, solid fueled fast breeder reactors need at least 8 tons of fissile fuel to start the reactor. While fast reactors can theoretically start up very well on the transuranic waste, their high fissile fuel startup makes this very expensive.[citation needed]
  • No downtime for refueling. LFTRs have liquid fuels, and therefore there is no need to shut down and take apart the reactor just to refuel it. LFTRs can thus refuel without causing a power outage (online refueling).
  • Load following. As the LFTR does not have xenon poisoning, there is no problem reducing the power in times of low demand for electricity and turn back on at any time.
  • No high pressure vessel. Since the core is not pressurized, it does not need the most expensive item in a light water reactor, a high-pressure reactor vessel for the core. Instead, there is a low-pressure vessel and pipes (for molten salt) constructed of relatively thin materials. Although the metal is an exotic nickel alloy that resists heat and corrosion, Hastelloy-N, the amount needed is relatively small.
  • Excellent heat transfer. Liquid fluoride salts, especially LiF based salts, have good heat transfer properties. Fuel salt such as LiF-ThF4 has a volumetric heat capacity that is around 22% higher than water,[64] FLiBe has around 12% higher heat capacity than water. In addition, the LiF based salts have a thermal conductivity around twice that of the hot pressurized water in a pressurized water reactor.[33][50] This results in efficient heat transfer and a compact primary loop. Compared to helium, a competing high temperature reactor coolant, the difference is even bigger. The fuel salt has over 200 times higher volumetric heat capacity as hot pressurized helium and over 3 times the thermal conductivity. A molten salt loop will use piping of 1/5 the diameter, and pumps 1/20 the power, of those required for high-pressure helium, while staying at atmospheric pressure[65]
  • Smaller, low pressure containment. By using liquid salt as the coolant instead of pressurized water, a containment structure only slightly bigger than the reactor vessel can be used. Light water reactors use pressurized water, which flashes to steam and expands a thousandfold in the case of a leak, necessitating a containment building a thousandfold bigger in volume than the reactor vessel. The LFTR containment can not only be smaller in physical size, its containment is also inherently low pressure. There are no sources of stored energy that could cause a rapid pressure rise (such as Hydrogen or steam) in the containment.[46][unreliable source] This gives the LFTR a substantial theoretical advantage not only in terms of inherent safety, but also in terms of smaller size, lower materials use, and lower construction cost.[8]
  • Air cooling. A high temperature power cycle can be air-cooled at little loss in efficiency,[66] which is critical for use in many regions where water is scarce. No need for large water cooling towers used in conventional steam-powered systems would also decrease power plant construction costs.[41][67]
  • From waste to resource. There are suggestions that it might be possible to extract some of the fission products so that they have separate commercial value.[68] However, compared to the produced energy, the value of the fission products is low, and chemical purification is expensive.[69]
  • Efficient mining. The extraction process of thorium from the earth's crust is a much safer and efficient mining method than that of uranium. Thorium’s ore, monazite, generally contains higher concentrations of thorium than the percentage of uranium found in its respective ore. This makes thorium a more cost efficient and less environmentally damaging fuel source. Thorium mining is also easier and less dangerous than uranium mining, as the mine is an open pit, which doesn't require ventilation such as the underground uranium mines, where radon levels are potentially harmful.[70]

Disadvantages

LFTRs are quite unlike today's operating commercial power reactors. These differences create design difficulties and trade-offs:
  • Highly questionable economics - although proponents of LFTR technology list a wide variety of claimed economic advantages, detailed studies of their economics invariably conclude there is no real advantage in overall terms. A number of the claims, like the ambient pressure operation and high-temperature cooling loops, are already used on a number of conventional designs and have failed to produce the economic gains claimed. In other cases, there is simply not enough data to justify any conclusion. When the entire development is considered, the conclusions are invariably something along the lines of one report's summary: "... the difference in cost, given the current industry environment, remains insufficient to justify the creation of a new LFTR."[71]
  • Reaching break even breeding is questionable - While the plans usually call for break even breeding, it is questionable if this is possible, when other requirements are to be met.[42] The thorium fuel cycle has on very little spare neutrons. Due to limited chemical reprocessing (for economic reasons) and compromises needed to achieve safety requirements like a negative void coefficient too many neutrons may be lost. Old proposed single fluid designs promising breeding performance tend to have an unsafe positive void coefficient and often assume excessive fuel cleaning to be economic viable.[42]
  • Still much development needed - Despite the ARE and MSRE experimental reactors already built in the 1960s, there is still a lot of development needed for the LFTR. This includes most of the chemical separation, (passive) emergency cooling, the tritium barrier, remote operated maintenance, large scale Li-7 production, the high temperature power cycle and more durable materials.
  • Startup fuel - Unlike mined uranium, mined thorium does not have a fissile isotope. Thorium reactors breed fissile uranium-233 from thorium, but require a small amount of fissile material for initial start up. There is relatively little of this material available. This raises the problem of how to start the reactors in a short time frame. One option is to produce U-233 in today's solid fueled reactors, then reprocess it out of the solid waste. An LFTR can also be started by other fissile isotopes, enriched uranium or plutonium from reactors or decommissioned bombs. For enriched uranium startup, high enrichment is needed. Decommissioned uranium bombs have enough enrichment, but not enough is available to start many LFTRs. It is difficult to separate plutonium fluoride from lanthanide fission products. One option for a two-fluid reactor is to operate with plutonium or enriched uranium in the fuel salt, breed U-233 in the blanket, and store it instead of returning it to the core. Instead, add plutonium or enriched uranium to continue the chain reaction, similar to today's solid fuel reactors. When enough U-233 is bred, replace the fuel with new fuel, retaining the U-233 for other startups. A similar option exists for a single-fluid reactor operating as a converter. Such a reactor would not reprocess fuel while operating. Instead the reactor would start on plutonium with thorium as the fertile and add plutonium. The plutonium eventually burns out and U-233 is produced in situ. At the end of the reactor fuel life, the spent fuel salt can be reprocessed to recover the bred U-233 to start up new LFTRs.[72]
  • Salts freezing - Fluoride salt mixtures have melting points ranging from 300 to 600 °C (572 to 1,112 °F). The salts, especially those with beryllium fluoride, are very viscous near their freezing point. This requires careful design and freeze protection in the containment and heat exchangers. Freezing must be prevented in normal operation, during transients, and during extended downtime. The primary loop salt contains the decay heat-generating fission products, which help to maintain the required temperature. For the MSBR, ORNL planned on keeping the entire reactor room (the hot cell) at high temperature. This avoided the need for individual electric heater lines on all piping and provided more even heating of the primary loop components.[18](p311) One "liquid oven" concept developed for molten salt-cooled, solid-fueled reactors employs a separate buffer salt pool containing the entire primary loop.[73] Because of the high heat capacity and considerable density of the buffer salt, the buffer salt prevents fuel salt freezing and participates in the passive decay heat cooling system, provides radiation shielding and reduces deadweight stresses on primary loop components. This design could also be adopted for LFTRs.[citation needed]
  • Beryllium toxicity - The proposed salt mixture FLiBe, contains large amounts of beryllium, which is toxic to humans (although nowhere near as toxic as the fission products and other radioactives). The salt in the primary cooling loops must be isolated from workers and the environment to prevent beryllium poisoning. This is routinely done in industry.[74](pp52–66) Based on this industrial experience, the added cost of beryllium safety is expected to cost only $0.12/MWh.[74](p61) After start up, the fission process in the primary fuel salt produces highly radioactive fission products with a high gamma and neutron radiation field. Effective containment is therefore a primary requirement. It is possible to operate instead using lithium fluoride-thorium fluoride eutectic without beryllium, as the French LFTR design, the "TMSR", has chosen.[75] This comes at the cost of a somewhat higher melting point, but has the additional advantages of simplicity (avoiding BeF
    2
    in the reprocessing systems), increased solubility for plutonium-trifluoride, reduced tritium production (beryllium produces lithium-6, which in turn produces tritium) and improved heat transfer (BeF
    2
    increases the viscosity of the salt mixture). Alternative solvents such as the fluorides of sodium, rubidium and zirconium allow lower melting points at a tradeoff in breeding.[1]
  • Loss of delayed neutrons - In order to be predictably controlled, nuclear reactors rely on delayed neutrons. They require additional slowly-evolving neutrons from fission product decay to continue the chain reaction. Because the delayed neutrons evolve slowly, this makes the reactor very controllable. In an LFTR, the presence of fission products in the heat exchanger and piping means a portion of these delayed neutrons are also lost.[76] They do not participate in the core's critical chain reaction, which in turn means the reactor behaves less gently during changes of flow, power, etc. Approximately up to half of the delayed neutrons can be lost. In practice, it means that the heat exchanger must be compact so that the volume outside the core is as small as possible. The more compact (higher power density) the core is, the more important this issue becomes. Having more fuel outside the core in the heat exchangers also means more of the expensive fissile fuel is needed to start the reactor. This makes a fairly compact heat exchanger an important design requirement for an LFTR.[citation needed]
  • Waste management - About 83% of the radioactive waste has a half-life in hours or days, with the remaining 17% requiring 300 year storage in geologically stable confinement to reach background levels.[63] Because some of the fission products, in their fluoride form, are highly water-soluble, fluorides are less suited to long-term storage. For example, cesium fluoride has a very high solubility in water. For long term storage, conversion to an insoluble form such as a glass, could be desirable.[citation needed]
  • Uncertain decommissioning costs - Cleanup of the Molten-Salt Reactor Experiment was about $130 million, for a small 8 MW(th) unit. Much of the high cost was caused by the unexpected evolution of fluorine and uranium hexafluoride from cold fuel salt in storage that ORNL did not defuel and store correctly, but this has now been taken into consideration in MSR design.[77] In addition, decommissioning costs don't scale strongly with plant size based on previous experience,[78] and costs are incurred at the end of plant life, so a small per kilowatthour fee is sufficient. For example, a GWe reactor plant produces over 300 billion kWh of electricity over a 40-year lifetime, so a $0.001/kWh decommissioning fee delivers $300 million plus interest at the end of the plant lifetime.
  • Noble metal buildup - Some radioactive fission products, such as noble metals, deposit on pipes. Novel equipment, such as nickel-wool sponge cartridges, must be developed to filter and trap the noble metals to prevent build up.
  • Limited graphite lifetime - Compact designs have a limited lifetime for the graphite moderator and fuel / breeding loop separator. Under the influence of fast neutrons, the graphite first shrinks, then expands indefinitely until it becomes very weak and can crack, creating mechanical problems and causing the graphite to absorb enough fission products to poison the reaction.[79] The 1960 two-fluid design had an estimated graphite replacement period of four years.[1](p3) Eliminating graphite from sealed piping was a major incentive to switch to a single-fluid design.[18](p3) Replacing this large central part requires remotely operated equipment. MSR designs have to arrange for this replacement. In a molten salt reactor, virtually all of the fuel and fission products can be piped to a holding tank. Only a fraction of one percent of the fission products end up in the graphite, primarily due to fission products slamming into the graphite. This makes the graphite surface radioactive, and without recycling/removal of at least the surface layer, creates a fairly bulky waste stream. Removing the surface layer and recycling the remainder of the graphite would solve this issue.[original research?] Several techniques exist to recycle or dispose of nuclear moderator graphite.[80] Graphite is inert and immobile at low temperatures, so it can be readily stored or buried if required.[80] At least one design used graphite balls (pebbles) floating in salt, which could be removed and inspected continuously without shutting down the reactor.[81] Reducing power density increases graphite lifetime.[82](p10) By comparison, solid-fueled reactors typically replace 1/3 of the fuel elements, including all of the highly radioactive fission products therein, every 12 to 24 months. This is routinely done under a protecting and cooling column layer of water.
  • Graphite-caused positive reactivity feedback - When graphite heats up, it increases U-233 fission, causing an undesirable positive feedback.[42] The LFTR design must avoid certain combinations of graphite and salt and certain core geometries. If this problem is addressed by employing adequate graphite and thus a well-thermalized spectrum, it is difficult to reach break-even breeding.[42] The alternative of using little or no graphite results in a faster neutron spectrum. This requires a large fissile inventory and radiation damage increases.[42]
  • Limited plutonium solubility - Fluorides of plutonium, americium and curium occur as trifluorides, which means they have three fluorine atoms attached (PuF
    3
    , AmF
    3
    , CmF
    3
    ). Such trifluorides have a limited solubility in the FLiBe carrier salt. This complicates startup, especially for a compact design that uses a smaller primary salt inventory. Of course, leaving plutonium carrying wastes out of the startup process is an even better solution, making this a non issue. Solubility can be increased by operating with less or no beryllium fluoride (which has no solubility for trifluorides) or by operating at a higher temperature[citation needed](as with most other liquids, solubility rises with temperature). A thermal spectrum, lower power density core does not have issues with plutonium solubility.
  • Proliferation risk from reprocessing - Effective reprocessing implies a proliferation risk. LFTRs could be used to handle plutonium from other reactors as well. However, as stated above, plutonium is chemically difficult to separate from thorium and plutonium cannot be used in bombs if diluted in large amounts of thorium. In addition, the plutonium produced by the thorium fuel cycle is mostly Pu-238, which produces high levels of spontaneous neutrons and decay heat that make it impossible to construct a fission bomb with this isotope alone, and extremely difficult to construct one containing even very small percentages of it. The heat production rate of 567 W/kg[83] means that a bomb core of this material would continuously produce several kilowatts of heat. The only cooling route is by conduction through the surrounding high explosive layers, which are poor conductors. This creates unmanageably high temperatures that would destroy the assembly. The spontaneous fission rate of 1204 kBq/g[83] is over twice that of Pu-240. Even very small percentages of this isotope would reduce bomb yield drastically by "predetonation" due to neutrons from spontaneous fission starting the chain reaction causing a "fizzle" rather than an explosion. Reprocessing itself involves automated handling in a fully closed and contained hot cell, which complicates diversion. Compared to today's extraction methods such as PUREX, the pyroprocesses are inaccessible and produce impure fissile materials, often with large amounts of fission product contamination. While not a problem for an automated system, it poses severe difficulties for would-be proliferators.[citation needed]
  • Proliferation risk from protactinium separation - Compact designs can breed only using rapid separation of protactinium, a proliferation risk, since this potentially gives access to high purity 233-U. This is difficult as the 233-U from these reactors will be contaminated with 232-U, a high gamma radiation emitter, requiring a protective hot enrichment facility[63] as a possible path to weapons-grade material. Because of this, commercial power reactors may have to be designed without separation. In practice, this means either not breeding, or operating at a lower power density. A two-fluid design might operate with a bigger blanket and keep the high power density core (which has no thorium and therefore no protactinium).[citation needed] However, a group of nuclear engineers argues in Nature (2012) that the protactinium pathway is feasible and that thorium is thus "not as benign as has been suggested . . ." [84]
  • Proliferation of neptunium-237 - In designs utilizing a fluorinator, Np-237 appears with uranium as gaseous hexafluoride and can be easily separated using solid fluoride pellet absorption beds. No one has produced such a bomb, but Np-237's considerable fast fission cross section and low critical mass imply the possibility.[85] When the Np-237 is kept in the reactor, it transmutes to short lived Pu-238. All reactors produce considerable neptunium, which is always present in high (mono)isotopic quality, and is easily extracted chemically.[85]
  • Neutron poisoning and tritium production from lithium-6 - Lithium-6 is a strong neutron poison; using LiF with natural lithium, with its 7.5% lithium-6 content, prevents reactors from starting. The high neutron density in the core rapidly transmutes lithium-6 to tritium, losing neutrons that are required to sustain break-even breeding. Tritium is a radioactive isotope of hydrogen, which is nearly identical, chemically, to ordinary hydrogen.[86] In the MSR the tritium is quite mobile because, in its elemental form, it rapidly diffuses through metals at high temperature. If the lithium is isotopically enriched in lithium-7, and the isotopic separation level is high enough (99.995% lithium-7), the amount of tritium produced is only a few hundred grams per year for a 1 GWe reactor. This much smaller amount of tritium comes mostly from the lithium-7 - tritium reaction and from beryllium, which can produce tritium indirectly by first transmuting to tritium-producing lithium-6. LFTR designs that use a lithium salt, choose the lithium-7 isotope. In the MSRE, lithium-6 was successfully removed from the fuel salt via isotopic enrichment. Since lithium-7 is at least 16% heavier than lithium-6, and is the most common isotope, lithium-6 is comparatively easy and inexpensive to extract. Vacuum distillation of lithium achieves efficiencies of up to 8% per stage and requires only heating in a vacuum chamber.[87] However, about one fission in 90,000 produces helium-6, which quickly decays to lithium-6 and one fission in 12,500 produces an atom of tritium directly (in all reactor types). Practical MSRs operate under a blanket of dry inert gas, usually helium. LFTRs offer a good chance to recover the tritium, since it is not highly diluted in water as in CANDU reactors. Various methods exist to trap tritium, such as hydriding it to titanium,[88] oxidizing it to less mobile (but still volatile) forms such as sodium fluoroborate or molten nitrate salt, or trapping it in the turbine power cycle gas and offgasing it using copper oxide pellets.[89](p41) ORNL developed a secondary loop coolant system that would chemically trap residual tritium so that it could be removed from the secondary coolant rather than diffusing into the turbine power cycle. ORNL calculated that this would reduce Tritium emissions to acceptable levels.[86]
  • Corrosion from tellurium - The reactor makes small amounts of tellurium as a fission product. In the MSRE, this caused small amounts of corrosion at the grain boundaries of the special nickel alloy, Hastelloy-N. Metallurgical studies showed that adding 1 to 2% niobium to the Hastelloy-N alloy improves resistance to corrosion by tellurium.[54](pp81–87) Maintaining the ratio of UF
    4
    /UF
    3
    to less than 60 reduced corrosion by keeping the fuel salt slightly reducing. The MSRE continually contacted the flowing fuel salt with a beryllium metal rod submerged in a cage inside the pump bowl. This caused a fluorine shortage in the salt, reducing tellurium to a less aggressive (elemental) form. This method is also effective in reducing corrosion in general, because the fission process produces more fluorine atoms that would otherwise attack the structural metals.[90](pp3–4)
  • Radiation damage to nickel alloys - The standard Hastelloy N alloy was found to be embrittled by neutron radiation. Neutrons reacted with nickel to form helium. This helium gas concentrated at specific points inside the alloy, where it increased stresses. ORNL addressed this problem by adding 1–2% titanium or niobium to the Hastelloy N. This changed the alloy's internal structure so that the helium would be finely distributed. This relieved the stress and allowed the alloy to withstand considerable neutron flux. However the maximum temperature is limited to about 650 °C.[91] Development of other alloys may be required.[92] The outer vessel wall that contains the salt can have neutronic shielding, such as boron carbide, to effectively protect it from neutron damage.[93]
  • Long term fuel salt storage - If the fluoride fuel salts are stored in solid form over many decades, radiation can cause the release of corrosive fluorine gas and uranium hexafluoride.[94] The salts must be defueled and wastes removed before extended shutdowns and stored above 100 degrees Celsius.[77] Fluorides are less suitable for long term storage because some have high water solubility unless vitrified in insoluble borosilicate glass.[95]
  • Business model - Today's solid-fueled reactor vendors make long term revenues by fuel fabrication.[dubious ] Without any fuel to fabricate and sell, an LFTR would adopt a different business model. There would be significant barrier to entry costs to make this a viable business. Existing infrastructure and parts suppliers are geared towards water-cooled reactors. There is little thorium market and thorium mining, so considerable infrastructure that would be required does not yet exist. Regulatory agencies have less experience regulating thorium reactors, creating potentials for extended delays.
  • Development of the power cycle - Developing a large helium or supercritical carbon dioxide turbine is needed for highest efficiency. These gas cycles offer numerous potential advantages for use with molten salt-fueled or molten salt-cooled reactors.[96] These closed gas cycles face design challenges and engineering upscaling work for a commercial turbine-generator set.[97] A standard supercritical steam turbine could be used at a small penalty in efficiency (the net efficiency of the MSBR was designed to be approximately 44%, using an old 1970s steam turbine).[98] A molten salt to steam generator would still have to be developed. Currently, molten nitrate salt steam generators are used in concentrated solar thermal power plants such as Andasol in Spain. Such a generator could be used for an MSR as a third circulating loop, where it would also trap any tritium that diffuses through the primary and secondary heat exchanger[99]

Recent developments

The Fuji MSR

The FUJI MSR was a design for a 100 to 200 MWe molten-salt-fueled thorium fuel cycle thermal breeder reactor, using technology similar to the Oak Ridge National Laboratory Reactor Experiment. It was being developed by a consortium including members from Japan, the United States, and Russia. As a breeder reactor, it converts thorium into nuclear fuels.[100] An industry group presented updated plans about FUJI MSR in July 2010.[101] They projected a cost of 2.85 cents per kilowatt hour.[102]

The IThEMS consortium planned to first build a much smaller MiniFUJI 10 MWe reactor of the same design once it had secured an additional $300 million in funding, but IThEMS closed in 2011 after it was unable to secure adequate funding. A new company, Thorium Tech Solution (TTS), was founded in 2011 by Kazuo Furukawa, the chief scientist from IThEMS, and Masaaki Furukawa. TTS acquired the FUJI design and some related patents.

Chinese thorium MSR project

The People's Republic of China has initiated a research and development project in thorium molten-salt reactor technology.[103] It was formally announced at the Chinese Academy of Sciences (CAS) annual conference in January 2011. Its ultimate target is to investigate and develop a thorium based molten salt nuclear system in about 20 years.[104][105] An expected intermediate outcome of the TMSR research program is to build a 2 MW pebble bed fluoride salt cooled research reactor in 2015, and a 2 MW molten salt fueled research reactor in 2017. This would be followed by a 10 MW demonstrator reactor and a 100 MW pilot reactors.[106][107] The project is spearheaded by Jiang Mianheng, with a start-up budget of $350 million, and has already recruited 140 PhD scientists, working full-time on thorium molten salt reactor research at the Shanghai Institute of Applied Physics. An expansion of staffing has increased to 700 as of 2015.[108] As of 2016, their plan is for a 10MW pilot LFTR is expected to be made operational in 2025, with a 100MW version set to follow in 2035.[109]

Flibe Energy

Kirk Sorensen, former NASA scientist and Chief Nuclear Technologist at Teledyne Brown Engineering, has been a long-time promoter of thorium fuel cycle and particularly liquid fluoride thorium reactors. He first researched thorium reactors while working at NASA, while evaluating power plant designs suitable for lunar colonies. Material about this fuel cycle was surprisingly hard to find, so in 2006 Sorensen started "energyfromthorium.com", a document repository, forum, and blog to promote this technology. In 2006, Sorensen coined the liquid fluoride thorium reactor and LFTR nomenclature to describe a subset of molten salt reactor designs based on liquid fluoride-salt fuels with breeding of thorium into uranium-233 in the thermal spectrum. In 2011, Sorensen founded Flibe Energy, a company that initially intends to develop 20-50 MW LFTR small modular reactor designs to power military bases. (It is easier to promote novel military designs than civilian power station designs in today's US nuclear regulatory environment).[110][111] An independent technology assessment coordinated with EPRI and Southern Company represents the most detailed information so far publicly available about Flibe Energy's proposed LFTR design.[112]

Thorium Energy Generation Pty. Limited (TEG)

Thorium Energy Generation Pty. Limited (TEG) was an Australian research and development company dedicated to the worldwide commercial development of LFTR reactors, as well as thorium accelerator-driven systems. As of June 2015, TEG had ceased operations.

Alvin Weinberg Foundation

The Alvin Weinberg Foundation is a British charity founded in 2011, dedicated to raising awareness about the potential of thorium energy and LFTR. It was formally launched at the House of Lords on 8 September 2011.[113][114][115] It is named after American nuclear physicist Alvin M. Weinberg, who pioneered the thorium molten salt reactor research.

Thorcon

Thorcon is a proposed molten salt converter reactor by Martingale, Florida. It features a simplified design with no reprocessing and swappable cans for ease of equipment replacement, in lieu of higher nuclear breeding efficiency.

Nuclear Research and Consultancy Group

On September 5, 2017, The Dutch Nuclear Research and Consultancy Group announced that research on the irradiation of molten thorium fluoride salts inside the Petten high-flux reactor was underway.[116]

Nuclear fuel cycle

From Wikipedia, the free encyclopedia

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 (or a once-through fuel cycle); if the spent fuel is reprocessed, it is referred to as a closed fuel cycle.

Basic concepts

Nuclear power relies on fissionable material that can sustain a chain reaction with neutrons. Examples of such materials include Uranium and Plutonium. Most nuclear reactors use a moderator to lower the kinetic energy of the neutrons and increase the probability that fission will occur. This allows reactors to use material with far lower concentration of fissile isotopes than are needed for nuclear weapons. Graphite and heavy water are the most effective moderators, because they slow the neutrons through collisions without absorbing them. Reactors using heavy water or graphite as the moderator can operate using natural uranium.

A light water reactor (LWR) uses water in the form that occurs in nature, and requires fuel enriched to higher concentrations of fissile isotopes. Typically, LWRs use uranium enriched to 3–5% content of the less common isotope U-235, the only fissile isotope that is found in significant quantity in nature. One alternative to this low-enriched uranium (LEU) fuel are mixed oxide (MOX) fuels produced by blending plutonium with natural or depleted uranium, and these fuels provide an avenue to utilize surplus weapons-grade plutonium. Another type of MOX fuel involves mixing LEU with thorium, which generates the fissile isotope U-233. Both plutonium and U-233 are produced from the absorption of neutrons by irradiating fertile materials in a reactor, in particular the common uranium isotope U-238 and thorium, respectively, and can be separated from spent uranium and thorium fuels in reprocessing plants.

Some reactors do not use moderators to slow the neutrons. Like nuclear weapons, which also use unmoderated or "fast" neutrons, these fast-neutron reactors require much higher concentrations of fissile isotopes in order to sustain a chain reaction. They are also capable of breeding fissile isotopes from fertile materials; a breeder reactor is one that generates more fissile material in this way than it consumes.

During the nuclear reaction inside a reactor, the fissile isotopes in nuclear fuel are consumed, producing more and more fission products, most of which are considered radioactive waste. The buildup of fission products and consumption of fissile isotopes eventually stop the nuclear reaction, causing the fuel to become a spent nuclear fuel. When 3% enriched LEU fuel is used, the spent fuel typically consists of roughly 1% U-235, 95% U-238, 1% plutonium and 3% fission products. Spent fuel and other high-level radioactive waste is extremely hazardous, although nuclear reactors produce relatively small volumes of waste compared to other power plants because of the high energy density of nuclear fuel. Safe management of these byproducts of nuclear power, including their storage and disposal, is a difficult problem for any country using nuclear power.

Front end

Exploration

A deposit of uranium, such as uraninite, discovered by geophysical techniques, is evaluated and sampled to determine the amounts of uranium materials that are extractable at specified costs from the deposit. Uranium reserves are the amounts of ore that are estimated to be recoverable at stated costs.

Naturally occurring uranium consists primarily of two isotopes U-238 and U-235, with 99.28% of the metal being U-238 while 0.71% is U-235, and the remaining 0.01% is mostly U-234. The number in such names refers to the isotope's atomic mass number, which is the number of protons plus the number of neutrons in the atomic nucleus.

The atomic nucleus of U-235 will nearly always fission when struck by a free neutron, and the isotope is therefore said to be a "fissile" isotope. The nucleus of a U-238 atom on the other hand, rather than undergoing fission when struck by a free neutron, will nearly always absorb the neutron and yield an atom of the isotope U-239. This isotope then undergoes natural radioactive decay to yield Pu-239, which, like U-235, is a fissile isotope. The atoms of U-238 are said to be fertile, because, through neutron irradiation in the core, some eventually yield atoms of fissile Pu-239.

Mining

Uranium ore can be extracted through conventional mining in open pit and underground methods similar to those used for mining other metals. In-situ leach mining methods also are used to mine uranium in the United States. In this technology, uranium is leached from the in-place ore through an array of regularly spaced wells and is then recovered from the leach solution at a surface plant. Uranium ores in the United States typically range from about 0.05 to 0.3% uranium oxide (U3O8). Some uranium deposits developed in other countries are of higher grade and are also larger than deposits mined in the United States. Uranium is also present in very low-grade amounts (50 to 200 parts per million) in some domestic phosphate-bearing deposits of marine origin. Because very large quantities of phosphate-bearing rock are mined for the production of wet-process phosphoric acid used in high analysis fertilizers and other phosphate chemicals, at some phosphate processing plants the uranium, although present in very low concentrations, can be economically recovered from the process stream.

Milling

Mined uranium ores normally are processed by grinding the ore materials to a uniform particle size and then treating the ore to extract the uranium by chemical leaching. The milling process commonly yields dry powder-form material consisting of natural uranium, "yellowcake", which is sold on the uranium market as U3O8. Note that the material isn't always yellow.

Uranium conversion

Usually milled Uranium oxide, U3O8 (Triuranium octaoxide) is then processed into either of 2 substances depending on the intended use.

For use in most reactors U3O8 is usually converted to Uranium hexafluoride (UF6), the input stock for most commercial uranium enrichment facilities. A solid at room temperature, uranium hexafluoride becomes gaseous at 57 °C (134 °F). At this stage of the cycle the uranium hexafluoride conversion product still has the natural isotopic mix (99.28% of U-238 plus 0.71% of U-235).

For use in reactors such as CANDU which do not require enriched fuel, the U3O8 may instead be converted to uranium dioxide (UO2) which can be included in ceramic fuel elements.

In the current nuclear industry the volume of material converted directly to UO2 is typically quite small compared to that converted to UF6.

Enrichment


Nuclear fuel cycle begins when uranium is mined, enriched and manufactured to nuclear fuel (1) which is delivered to a nuclear power plant. After usage in the power plant the spent fuel is delivered to a reprocessing plant (if fuel is recycled) (2) or to a final repository (if no recycling is done) (3) for geological disposition. In reprocessing 95% of spent fuel can be recycled to be returned to usage in a nuclear power plant (4).

The natural concentration (0.71%) of the fissionable isotope U-235 is less than that required to sustain a nuclear chain reaction in light water reactor cores. Accordingly UF6 produced from natural Uranium sources must be enriched to a higher concentration of the fissionable isotope before being used as nuclear fuel in such reactors. The level of enrichment for a particular nuclear fuel order is specified by the customer according to the application they will use it for: light-water reactor fuel normally is enriched to 3.5% U-235, but uranium enriched to lower concentrations is also required. Enrichment is accomplished using any of several methods of isotope separation. Gaseous diffusion and gas centrifuge are the commonly used uranium enrichment methods, but new enrichment technologies are currently being developed.

The bulk (96%) of the byproduct from enrichment is depleted uranium (DU), which can be used for armor, kinetic energy penetrators, radiation shielding and ballast. As of 2008 there are vast quantities of depleted uranium in storage. The United States Department of Energy alone has 470,000 tonnes.[1] About 95% of depleted uranium is stored as uranium hexafluoride (UF6).

Fabrication

For use as nuclear fuel, enriched uranium hexafluoride is converted into uranium dioxide (UO2) powder that is then processed into pellet form. The pellets are then fired in a high temperature sintering furnace to create hard, ceramic pellets of enriched uranium. The cylindrical pellets then undergo a grinding process to achieve a uniform pellet size. The pellets are stacked, according to each nuclear reactor core's design specifications, into tubes of corrosion-resistant metal alloy. The tubes are sealed to contain the fuel pellets: these tubes are called fuel rods. The finished fuel rods are grouped in special fuel assemblies that are then used to build up the nuclear fuel core of a power reactor.
The alloy used for the tubes depends on the design of the reactor. Stainless steel was used in the past, but most reactors now use a zirconium alloy. For the most common types of reactors, boiling water reactors (BWR) and pressurized water reactors (PWR), the tubes are assembled into bundles[2] with the tubes spaced precise distances apart. These bundles are then given a unique identification number, which enables them to be tracked from manufacture through use and into disposal.

Service period

Transport of radioactive materials

Transport is an integral part of the nuclear fuel cycle. There are nuclear power reactors in operation in several countries but uranium mining is viable in only a few areas. Also, in the course of over forty years of operation by the nuclear industry, a number of specialized facilities have been developed in various locations around the world to provide fuel cycle services and there is a need to transport nuclear materials to and from these facilities.[3] Most transports of nuclear fuel material occur between different stages of the cycle, but occasionally a material may be transported between similar facilities. With some exceptions, nuclear fuel cycle materials are transported in solid form, the exception being uranium hexafluoride (UF6) which is considered a gas. Most of the material used in nuclear fuel is transported several times during the cycle. Transports are frequently international, and are often over large distances. Nuclear materials are generally transported by specialized transport companies.

Since nuclear materials are radioactive, it is important to ensure that radiation exposure of those involved in the transport of such materials and of the general public along transport routes is limited. Packaging for nuclear materials includes, where appropriate, shielding to reduce potential radiation exposures. In the case of some materials, such as fresh uranium fuel assemblies, the radiation levels are negligible and no shielding is required. Other materials, such as spent fuel and high-level waste, are highly radioactive and require special handling. To limit the risk in transporting highly radioactive materials, containers known as spent nuclear fuel shipping casks are used which are designed to maintain integrity under normal transportation conditions and during hypothetical accident conditions.

In-core fuel management

A nuclear reactor core is composed of a few hundred "assemblies", arranged in a regular array of cells, each cell being formed by a fuel or control rod surrounded, in most designs, by a moderator and coolant, which is water in most reactors.

Because of the fission process that consumes the fuels, the old fuel rods must be replaced periodically with fresh ones (this is called a (replacement) cycle). During a given replacement cycle only some of the assemblies (typically one-third) are replaced since fuel depletion occurs at different rates at different places within the reactor core. Furthermore, for efficiency reasons, it is not a good policy to put the new assemblies exactly at the location of the removed ones. Even bundles of the same age will have different burn-up levels due to their previous positions in the core. Thus the available bundles must be arranged in such a way that the yield is maximized, while safety limitations and operational constraints are satisfied. Consequently, reactor operators are faced with the so-called optimal fuel reloading problem, which consists of optimizing the rearrangement of all the assemblies, the old and fresh ones, while still maximizing the reactivity of the reactor core so as to maximise fuel burn-up and minimise fuel-cycle costs.

This is a discrete optimization problem, and computationally infeasible by current combinatorial methods, due to the huge number of permutations and the complexity of each computation. Many numerical methods have been proposed for solving it and many commercial software packages have been written to support fuel management. This is an ongoing issue in reactor operations as no definitive solution to this problem has been found. Operators use a combination of computational and empirical techniques to manage this problem.

The study of used fuel

Used nuclear fuel is studied in Post irradiation examination, where used fuel is examined to know more about the processes that occur in fuel during use, and how these might alter the outcome of an accident. For example, during normal use, the fuel expands due to thermal expansion, which can cause cracking. Most nuclear fuel is uranium dioxide, which is a cubic solid with a structure similar to that of calcium fluoride. In used fuel the solid state structure of most of the solid remains the same as that of pure cubic uranium dioxide. SIMFUEL is the name given to the simulated spent fuel which is made by mixing finely ground metal oxides, grinding as a slurry, spray drying it before heating in hydrogen/argon to 1700 oC.[4] In SIMFUEL, 4.1% of the volume of the solid was in the form of metal nanoparticles which are made of molybdenum, ruthenium, rhodium and palladium. Most of these metal particles are of the ε phase (hexagonal) of Mo-Ru-Rh-Pd alloy, while smaller amounts of the α (cubic) and σ (tetragonal) phases of these metals were found in the SIMFUEL. Also present within the SIMFUEL was a cubic perovskite phase which is a barium strontium zirconate (BaxSr1−xZrO3).

The solid state structure of uranium dioxide, the oxygen atoms are in green and the uranium atoms in red

Uranium dioxide is very insoluble in water, but after oxidation it can be converted to uranium trioxide or another uranium(VI) compound which is much more soluble. Uranium dioxide (UO2) can be oxidised to an oxygen rich hyperstoichiometric oxide (UO2+x) which can be further oxidised to U4O9, U3O7, U3O8 and UO3.2H2O.

Because used fuel contains alpha emitters (plutonium and the minor actinides), the effect of adding an alpha emitter (238Pu) to uranium dioxide on the leaching rate of the oxide has been investigated. For the crushed oxide, adding 238Pu tended to increase the rate of leaching, but the difference in the leaching rate between 0.1 and 10% 238Pu was very small.[5]

The concentration of carbonate in the water which is in contact with the used fuel has a considerable effect on the rate of corrosion, because uranium(VI) forms soluble anionic carbonate complexes such as [UO2(CO3)2]2− and [UO2(CO3)3]4−. When carbonate ions are absent, and the water is not strongly acidic, the hexavalent uranium compounds which form on oxidation of uranium dioxide often form insoluble hydrated uranium trioxide phases.[6]

Thin films of uranium dioxide can be deposited upon gold surfaces by ‘sputtering’ using uranium metal and an argon/oxygen gas mixture. These gold surfaces modified with uranium dioxide have been used for both cyclic voltammetry and AC impedance experiments, and these offer an insight into the likely leaching behaviour of uranium dioxide.[7]

Fuel cladding interactions

The study of the nuclear fuel cycle includes the study of the behaviour of nuclear materials both under normal conditions and under accident conditions. For example, there has been much work on how uranium dioxide based fuel interacts with the zirconium alloy tubing used to cover it. During use, the fuel swells due to thermal expansion and then starts to react with the surface of the zirconium alloy, forming a new layer which contains both fuel and zirconium (from the cladding). Then, on the fuel side of this mixed layer, there is a layer of fuel which has a higher caesium to uranium ratio than most of the fuel. This is because xenon isotopes are formed as fission products that diffuse out of the lattice of the fuel into voids such as the narrow gap between the fuel and the cladding. After diffusing into these voids, it decays to caesium isotopes. Because of the thermal gradient which exists in the fuel during use, the volatile fission products tend to be driven from the centre of the pellet to the rim area.[8] Below is a graph of the temperature of uranium metal, uranium nitride and uranium dioxide as a function of distance from the centre of a 20 mm diameter pellet with a rim temperature of 200 oC. The uranium dioxide (because of its poor thermal conductivity) will overheat at the centre of the pellet, while the other more thermally conductive forms of uranium remain below their melting points.


Temperature profile for a 20 mm diameter fuel pellet with a
power density of 1 kW per cubic meter. The fuels other than
uranium dioxide are not compromised.

Normal and abnormal conditions

The nuclear chemistry associated with the nuclear fuel cycle can be divided into two main areas; one area is concerned with operation under the intended conditions while the other area is concerned with maloperation conditions where some alteration from the normal operating conditions has occurred or (more rarely) an accident is occurring.

The releases of radioactivity from normal operations are the small planned releases from uranium ore processing, enrichment, power reactors, reprocessing plants and waste stores. These can be in different chemical/physical form from releases which could occur under accident conditions. In addition the isotope signature of a hypothetical accident may be very different from that of a planned normal operational discharge of radioactivity to the environment.

Just because a radioisotope is released it does not mean it will enter a human and then cause harm. For instance, the migration of radioactivity can be altered by the binding of the radioisotope to the surfaces of soil particles. For example, caesium (Cs) binds tightly to clay minerals such as illite and montmorillonite, hence it remains in the upper layers of soil where it can be accessed by plants with shallow roots (such as grass). Hence grass and mushrooms can carry a considerable amount of 137Cs which can be transferred to humans through the food chain. But 137Cs is not able to migrate quickly through most soils and thus is unlikely to contaminate well water. Colloids of soil minerals can migrate through soil so simple binding of a metal to the surfaces of soil particles does not completely fix the metal.

According to Jiří Hála's text book, the distribution coefficient Kd is the ratio of the soil's radioactivity (Bq g−1) to that of the soil water (Bq ml−1). If the radioisotope is tightly bound to the minerals in the soil, then less radioactivity can be absorbed by crops and grass growing on the soil.
In dairy farming, one of the best countermeasures against 137Cs is to mix up the soil by deeply ploughing the soil. This has the effect of putting the 137Cs out of reach of the shallow roots of the grass, hence the level of radioactivity in the grass will be lowered. Also after a nuclear war or serious accident, the removal of top few cm of soil and its burial in a shallow trench will reduce the long-term gamma dose to humans due to 137Cs, as the gamma photons will be attenuated by their passage through the soil.

Even after the radioactive element arrives at the roots of the plant, the metal may be rejected by the biochemistry of the plant. The details of the uptake of 90Sr and 137Cs into sunflowers grown under hydroponic conditions has been reported.[9] The caesium was found in the leaf veins, in the stem and in the apical leaves. It was found that 12% of the caesium entered the plant, and 20% of the strontium. This paper also reports details of the effect of potassium, ammonium and calcium ions on the uptake of the radioisotopes.

In livestock farming, an important countermeasure against 137Cs is to feed animals a small amount of Prussian blue. This iron potassium cyanide compound acts as an ion-exchanger. The cyanide is so tightly bonded to the iron that it is safe for a human to eat several grams of Prussian blue per day. The Prussian blue reduces the biological half-life (different from the nuclear half-life) of the caesium. The physical or nuclear half-life of 137Cs is about 30 years. This is a constant which can not be changed but the biological half-life is not a constant. It will change according to the nature and habits of the organism for which it is expressed. Caesium in humans normally has a biological half-life of between one and four months. An added advantage of the Prussian blue is that the caesium which is stripped from the animal in the droppings is in a form which is not available to plants. Hence it prevents the caesium from being recycled. The form of Prussian blue required for the treatment of humans or animals is a special grade. Attempts to use the pigment grade used in paints have not been successful. Note that a good[according to whom?] source of data on the subject of caesium in Chernobyl fallout exists at [1] (Ukrainian Research Institute for Agricultural Radiology).
Release of radioactivity from fuel during normal use and accidents
The IAEA assume that under normal operation the coolant of a water-cooled reactor will contain some radioactivity[10] but during a reactor accident the coolant radioactivity level may rise. The IAEA states that under a series of different conditions different amounts of the core inventory can be released from the fuel, the four conditions the IAEA consider are normal operation, a spike in coolant activity due to a sudden shutdown/loss of pressure (core remains covered with water), a cladding failure resulting in the release of the activity in the fuel/cladding gap (this could be due to the fuel being uncovered by the loss of water for 15–30 minutes where the cladding reached a temperature of 650-1250 oC) or a melting of the core (the fuel will have to be uncovered for at least 30 minutes, and the cladding would reach a temperature in excess of 1650 oC).[11]

Based upon the assumption that a Pressurized water reactor contains 300 tons of water, and that the activity of the fuel of a 1 GWe reactor is as the IAEA predicts,[12] then the coolant activity after an accident such as the Three Mile Island accident (where a core is uncovered and then recovered with water) can be predicted.[citation needed]
Releases from reprocessing under normal conditions
It is normal to allow used fuel to stand after the irradiation to allow the short-lived and radiotoxic iodine isotopes to decay away. In one experiment in the USA, fresh fuel which had not been allowed to decay was reprocessed (the Green run [2] [3] [4]) to investigate the effects of a large iodine release from the reprocessing of short cooled fuel. It is normal in reprocessing plants to scrub the off gases from the dissolver to prevent the emission of iodine. In addition to the emission of iodine the noble gases and tritium are released from the fuel when it is dissolved. It has been proposed that by voloxidation (heating the fuel in a furnace under oxidizing conditions) the majority of the tritium can be recovered from the fuel.[5]

A paper was written on the radioactivity in oysters found in the Irish Sea.[13] These were found by gamma spectroscopy to contain 141Ce, 144Ce, 103Ru, 106Ru, 137Cs, 95Zr and 95Nb. Additionally, a zinc activation product (65Zn) was found, which is thought to be due to the corrosion of magnox fuel cladding in spent fuel pools. It is likely that the modern releases of all these isotopes from the Windscale event is smaller.

On-load reactors

Some reactor designs, such as RBMKs or CANDU reactors, can be refueled without being shut down. This is achieved through the use of many small pressure tubes to contain the fuel and coolant, as opposed to one large pressure vessel as in pressurized water reactor (PWR) or boiling water reactor (BWR) designs. Each tube can be individually isolated and refueled by an operator-controlled fueling machine, typically at a rate of up to 8 channels per day out of roughly 400 in CANDU reactors. On-load refueling allows for the optimal fuel reloading problem to be dealt with continuously, leading to more efficient use of fuel. This increase in efficiency is partially offset by the added complexity of having hundreds of pressure tubes and the fueling machines to service them.

Interim storage

After its operating cycle, the reactor is shut down for refueling. The fuel discharged at that time (spent fuel) is stored either at the reactor site (commonly in a spent fuel pool) or potentially in a common facility away from reactor sites. If on-site pool storage capacity is exceeded, it may be desirable to store the now cooled aged fuel in modular dry storage facilities known as Independent Spent Fuel Storage Installations (ISFSI) at the reactor site or at a facility away from the site. The spent fuel rods are usually stored in water or boric acid, which provides both cooling (the spent fuel continues to generate decay heat as a result of residual radioactive decay) and shielding to protect the environment from residual ionizing radiation, although after at least a year of cooling they may be moved to dry cask storage.

Reprocessing

Spent fuel discharged from reactors contains appreciable quantities of fissile (U-235 and Pu-239), fertile (U-238), and other radioactive materials, including reaction poisons, which is why the fuel had to be removed. These fissile and fertile materials can be chemically separated and recovered from the spent fuel. The recovered uranium and plutonium can, if economic and institutional conditions permit, be recycled for use as nuclear fuel. This is currently not done for civilian spent nuclear fuel in the United States.

Mixed oxide, or MOX fuel, is a blend of reprocessed uranium and plutonium and depleted uranium which behaves similarly, although not identically, to the enriched uranium feed for which most nuclear reactors were designed. MOX fuel is an alternative to low-enriched uranium (LEU) fuel used in the light water reactors which predominate nuclear power generation.

Currently, plants in Europe are reprocessing spent fuel from utilities in Europe and Japan. Reprocessing of spent commercial-reactor nuclear fuel is currently not permitted in the United States due to the perceived danger of nuclear proliferation. However, the recently announced Global Nuclear Energy Partnership would see the U.S. form an international partnership to see spent nuclear fuel reprocessed in a way that renders the plutonium in it usable for nuclear fuel but not for nuclear weapons.

Partitioning and transmutation

As an alternative to the disposal of the PUREX raffinate in glass or Synroc matrix, the most radiotoxic elements could be removed through advanced reprocessing. After separation, the minor actinides and some long-lived fission products could be converted to short-lived or stable isotopes by either neutron or photon irradiation. This is called transmutation. However, a strong and long-term international cooperation, many decades of research and huge investments remain necessary before to reach a mature industrial scale where the safety and the economical feasibility of partitioning and transmutation (P&T) could be demonstrated.[14]

Waste disposal

A current concern in the nuclear power field is the safe disposal and isolation of either spent fuel from reactors or, if the reprocessing option is used, wastes from reprocessing plants. These materials must be isolated from the biosphere until the radioactivity contained in them has diminished to a safe level.[20] In the U.S., under the Nuclear Waste Policy Act of 1982 as amended, the Department of Energy has responsibility for the development of the waste disposal system for spent nuclear fuel and high-level radioactive waste. Current plans call for the ultimate disposal of the wastes in solid form in a licensed deep, stable geologic structure called a deep geological repository. The Department of Energy chose Yucca Mountain as the location for the repository. However, its opening has been repeatedly delayed. Since 1999 thousands of nuclear waste shipments have been stored at the Waste Isolation Pilot Plant in New Mexico.

Fast-neutron reactors can fission all actinides, while the thorium fuel cycle produces low levels of transuranics. Unlike LWRs, in principle these fuel cycles could recycle their plutonium and minor actinides and leave only fission products and activation products as waste. The highly radioactive medium-lived fission products Cs-137 and Sr-90 diminish by a factor of 10 each century; while the long-lived fission products have relatively low radioactivity, often compared favorably to that of the original uranium ore.

Fuel cycles

Although the most common terminology is fuel cycle, some argue that the term fuel chain is more accurate, because the spent fuel is never fully recycled. Spent fuel includes fission products, which generally must be treated as waste, as well as uranium, plutonium, and other transuranic elements. Where plutonium is recycled, it is normally reused once in light water reactors, although fast reactors could lead to more complete recycling of plutonium.[21]

Once-through nuclear fuel cycle


A once through (or open) fuel cycle

Not a cycle per se, fuel is used once and then sent to storage without further processing save additional packaging to provide for better isolation from the biosphere. This method is favored by six countries: the United States, Canada, Sweden, Finland, Spain and South Africa.[22] Some countries, notably Finland, Sweden and Canada, have designed repositories to permit future recovery of the material should the need arise, while others plan for permanent sequestration in a geological repository like the Yucca Mountain nuclear waste repository in the United States.

Plutonium cycle


A fuel cycle in which plutonium is used for fuel

The integral fast reactor concept (color), with the reactor above and integrated pyroprocessing fuel cycle below. A more detailed animation and demonstration is available.[23]

IFR concept (Black and White with clearer text)

Several countries, including Japan, Switzerland, and previously Spain and Germany,[citation needed] are using or have used the reprocessing services offered by BNFL and COGEMA. Here, the fission products, minor actinides, activation products, and reprocessed uranium are separated from the reactor-grade plutonium, which can then be fabricated into MOX fuel. Because the proportion of the non-fissile even-mass isotopes of plutonium rises with each pass through the cycle, there are currently no plans to reuse plutonium from used MOX fuel for a third pass in a thermal reactor. However, if fast reactors become available, they may be able to burn these, or almost any other actinide isotopes.

The use of a medium-scale reprocessing facility onsite, and the use of pyroprocessing rather than the present day aqueous reprocessing, is claimed to considerably reduce the proliferation potential or possible diversion of fissile material as the processing facility is in-situ/integral. Similarly as plutonium is not seperated on its own in the pyroprocessing cycle, rather all actinides are "electro-won" or "refined" from the spent fuel, the plutonium is never separated on its own, instead it comes over into the new fuel mixed with gamma and alpha emitting actinides, species that "self-protect" it in numerous possible thief scenarios.

Minor actinides recycling

It has been proposed that in addition to the use of plutonium, the minor actinides could be used in a critical power reactor. Tests are already being conducted in which americium is being used as a fuel.[24]

A number of reactor designs, like the Integral Fast Reactor, have been designed for this rather different fuel cycle. In principle, it should be possible to derive energy from the fission of any actinide nucleus. With a careful reactor design, all the actinides in the fuel can be consumed, leaving only lighter elements with short half-lives. Whereas this has been done in prototype plants, no such reactor has ever been operated on a large scale.[citation needed]

It so happens that the neutron cross-section of many actinides decreases with increasing neutron energy, but the ratio of fission to simple activation (neutron capture) changes in favour of fission as the neutron energy increases. Thus with a sufficiently high neutron energy, it should be possible to destroy even curium without the generation of the transcurium metals. This could be very desirable as it would make it significantly easier to reprocess and handle the actinide fuel.

One promising alternative from this perspective is an accelerator-driven sub-critical reactor / subcritical reactor. Here a beam of either protons (United States and European designs)[25][26][27] or electrons (Japanese design)[28] is directed into a target. In the case of protons, very fast neutrons will spall off the target, while in the case of the electrons, very high energy photons will be generated. These high-energy neutrons and photons will then be able to cause the fission of the heavy actinides.

Such reactors compare very well to other neutron sources in terms of neutron energy:
As an alternative, the curium-244, with a half-life of 18 years, could be left to decay into plutonium-240 before being used in fuel in a fast reactor.


 A pair of fuel cycles in which uranium and plutonium are kept
separate from the minor actinides. The minor actinide cycle is
kept within the green box.

Fuel or targets for this actinide transmutation

To date the nature of the fuel (targets) for actinide transformation has not been chosen.

If actinides are transmuted in a Subcritical reactor, it is likely that the fuel will have to be able to tolerate more thermal cycles than conventional fuel. An accelerator-driven sub-critical reactor is unlikely to be able to maintain a constant operation period for equally long times as a critical reactor, and each time the accelerator stops then the fuel will cool down.

On the other hand, if actinides are destroyed using a fast reactor, such as an Integral Fast Reactor, then the fuel will most likely not be exposed to many more thermal cycles than in a normal power station.

Depending on the matrix the process can generate more transuranics from the matrix. This could either be viewed as good (generate more fuel) or can be viewed as bad (generation of more radiotoxic transuranic elements). A series of different matrices exists which can control this production of heavy actinides.

Fissile nuclei, like Uranium-235, Plutonium-239 and Uranium-233 respond well to delayed neutrons and are thus important to keep a critical reactor stable, and this limits the amount of minor actinides that can be destroyed in a critical reactor. As a consequence, it is important that the chosen matrix allows the reactor to keep the ratio of fissile to non-fissile nuclei high, as this enables it to destroy the long-lived actinides safely. In contrast, the power output of a sub-critical reactor is limited by the intensity of the driving particle accelerator, and thus it need not contain any uranium or plutonium at all. In such a system, it may be preferable to have an inert matrix that doesn't produce additional long-lived isotopes.
Actinides in an inert matrix
The actinides will be mixed with a metal which will not form more actinides, for instance an alloy of actinides in a solid such as zirconia could be used.
Actinides in a thorium matrix
Thorium will on neutron bombardment form uranium-233. U-233 is fissile, and has a larger fission cross section than both U-235 and U-238, and thus it is far less likely to produce higher actinides through neutron capture.
Actinides in a uranium matrix
If the actinides are incorporated into a uranium-metal or uranium-oxide matrix, then the neutron capture of U-238 is likely to generate new plutonium-239. An advantage of mixing the actinides with uranium and plutonium is that the large fission cross sections of U-235 and Pu-239 for the less energetic delayed-neutrons could make the reaction stable enough to be carried out in a critical fast reactor, which is likely to be both cheaper and simpler than an accelerator driven system.
Mixed matrix
It is also possible to create a matrix made from a mix of the above-mentioned materials. This is most commonly done in fast reactors where one may wish to keep the breeding ratio of new fuel high enough to keep powering the reactor, but still low enough that the generated actinides can be safely destroyed without transporting them to another site. One way to do this is to use fuel where actinides and uranium is mixed with inert zirconium, producing fuel elements with the desired properties.

Thorium cycle

In the thorium fuel cycle thorium-232 absorbs a neutron in either a fast or thermal reactor. The thorium-233 beta decays to protactinium-233 and then to uranium-233, which in turn is used as fuel. Hence, like uranium-238, thorium-232 is a fertile material.
{\displaystyle {\ce {{\overset {neutron}{n}}+{^{232}_{90}Th}->{^{233}_{90}Th}->[\beta ^{-}]{^{233}_{91}Pa}->[\beta ^{-}]{\overset {fuel}{^{233}_{92}U}}}}}
After starting the reactor with existing U-233 or some other fissile material such as U-235 or Pu-239, a breeding cycle similar to but more efficient[29] than that with U-238 and plutonium can be created. The Th-232 absorbs a neutron to become Th-233 which quickly decays to protactinium-233. Protactinium-233 in turn decays with a half-life of 27 days to U-233. In some molten salt reactor designs, the Pa-233 is extracted and protected from neutrons (which could transform it to Pa-234 and then to U-234), until it has decayed to U-233. This is done in order to improve the breeding ratio which is low compared to fast reactors.

Thorium is at least 4-5 times more abundant in nature than all of uranium isotopes combined; thorium is fairly evenly spread around Earth with a lot of countries[30] having huge supplies of it; preparation of thorium fuel does not require difficult [29] and expensive enrichment processes; the thorium fuel cycle creates mainly Uranium-233 contaminated with Uranium-232 which makes it harder to use in a normal, pre-assembled nuclear weapon which is stable over long periods of time (unfortunately drawbacks are much lower for immediate use weapons or where final assembly occurs just prior to usage time); elimination of at least the transuranic portion of the nuclear waste problem is possible in MSR and other breeder reactor designs.

One of the earliest efforts to use a thorium fuel cycle took place at Oak Ridge National Laboratory in the 1960s. An experimental reactor was built based on molten salt reactor technology to study the feasibility of such an approach, using thorium fluoride salt kept hot enough to be liquid, thus eliminating the need for fabricating fuel elements. This effort culminated in the Molten-Salt Reactor Experiment that used 232Th as the fertile material and 233U as the fissile fuel. Due to a lack of funding, the MSR program was discontinued in 1976.

Current industrial activity

Currently the only isotopes used as nuclear fuel are uranium-235 (U-235), uranium-238 (U-238) and plutonium-239, although the proposed thorium fuel cycle has advantages. Some modern reactors, with minor modifications, can use thorium. Thorium is approximately three times more abundant in the Earth's crust than uranium (and 550 times more abundant than uranium-235). However, there has been little exploration for thorium resources, and thus the proved resource is small. Thorium is more plentiful than uranium in some countries, notably India.[31]

Heavy water reactors and graphite-moderated reactors can use natural uranium, but the vast majority of the world's reactors require enriched uranium, in which the ratio of U-235 to U-238 is increased. In civilian reactors, the enrichment is increased to as much as 5% U-235 and 95% U-238, but in naval reactors there is as much as 93% U-235.

The term nuclear fuel is not normally used in respect to fusion power, which fuses isotopes of hydrogen into helium to release energy.

Operator (computer programming)

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