Depleted uranium hexafluoride

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Depleted uranium hexafluoride (DUHF; also referred to as depleted uranium tails, depleted uranium tailings or DUF6) is a byproduct of the processing of uranium hexafluoride into enriched uranium. [1] [2] It is one of the chemical forms of depleted uranium (up to 73-75%), along with depleted triuranium octoxide (up to 25%) and depleted uranium metal (up to 2%). [3] [4] [5] [6] DUHF is 1.7 times less radioactive than uranium hexafluoride and natural uranium. [4]

Contents

History

The concept of depleted and enriched uranium emerged nearly 150 years after the discovery of uranium by Martin Klaproth in 1789. In 1938, two German physicists Otto Hahn and Fritz Strassmann had made the discovery of the fission of the atomic nucleus of the 235 U isotope, which was theoretically substantiated by Lise Meitner, Otto Robert Frisch and in parallel with them Gottfried von Droste and Siegfried Flügge. [7] [8] [9] This discovery marked the beginning of the peaceful and military use of the nuclear energy of uranium. [10] A year later, Yulii Khariton and Yakov Zeldovich were the first to prove theoretically that with an enrichment of 235U in natural uranium, a chain reaction could be sustained. [11] This nuclear chain reaction requires on average that at least one neutron, released by the fission of an atom of 235U, will be captured by another atom of 235U and will cause it also to fission. The probability of a neutron being captured by a fissile nucleus should be high enough to sustain the reaction. To increase this probability, an increase in the proportion of 235U is necessary, which in natural uranium constitutes only 0.72%, along with 99.27% 238 U and 0.0055% 234 U.

Competition

By the mid-1960s, the United States had a monopoly on the supply of uranium fuel for Western nuclear power plants. [12] In 1968, the USSR declared its readiness to accept orders for uranium enrichment. [13] As a result, a competitive market formed in the world, and commercial enrichment companies began to appear (e.g., URENCO and Eurodif). In 1971, the first Soviet contract was signed with the French Alternative Energies and Atomic Energy Commission, where nuclear power plants were actively built. In 1973, roughly 10 long-term contracts were signed with power companies from Italy, Germany, Great Britain, Spain, Sweden, Finland, Belgium and Switzerland. [14] By 2017, large commercial enrichment plants have been operating in France, Germany, the Netherlands, Great Britain, the United States, Russia and China. [15] The development of the enrichment market has led to the accumulation of over 2 million tons of DUHF in the world during this period. [16]

Other forms of depleted uranium

Depleted uranium may exist in several chemical forms; in the form of DUHF, the most common form, with a density of 5.09 g/cm3, in the form of depleted triuranium octoxide (U3O8) with a density of 8.38 g/cm3, and in the form of depleted uranium metal with a density of 19.01 g/cm3. [17]

Physical properties

Since the various uranium isotopes share the same chemical properties, the chemical and physical properties of depleted, enriched, and unenriched UF6 are identical, except for the degree of radioactivity. Like other forms of UF6, under standard conditions, DUHF forms white crystals, with a density of 5.09 g/cm3. At pressures below 1.5 atm, the solid DUHF sublimes into gas when heated, with no liquid form. At 1 atm, the sublimation point is 56.5 °C. The critical temperature of DUHF is 230.2 °C, and the critical pressure is 4.61 MPa.

Radioactivity

The radioactivity of DUHF is determined by the isotopic composition of uranium because the fluorine in the compound is stable. The radioactive decay rate of natural UF6 (with 0.72% 235U) is 1.7×104 Bq/g of which 97.6% is due to 238U and 234U.

Properties and contribution to the radioactivity of natural uranium of its isotopes [4]
Uranium isotope Mass fraction in natural uranium Half-life, yearsActivity of 1 mg of pure isotopeContribution to the activity of natural uranium
238U99.27%4.51×10912.4 Bq48.8%
235U0.72%7.04×10880 Bq2.4%
234U0.0055%2.45×105231000 Bq48.8%

When uranium is enriched, the content of light isotopes, 234U and 235U, increases. Although 234U, despite its much lower mass fraction, contributes more to the activity, the target isotope for nuclear industry use is 235U. Therefore, the degree of uranium enrichment or depletion is specified by the content of 235U. The reduction of 234U, and to a slight degree 235U, content reduces the radioactivity below unenriched UF6.

Radioactive decay rates of natural and depleted uranium hexafluoride depending on the level of enrichment [18]
Type of uranium hexafluorideDegree of 235U contentRadioactive decay rate, Bq/g [lower-alpha 1] Activity with respect to natural uranium hexafluoride
Natural

(with natural composition of uranium isotopes)

0,72%1,7×104100%
Depleted0,45%1,2×10470%


Production

Illustration of the uranium hexafluoride enrichment process Uranium Hexafluoride Enrichment.svg
Illustration of the uranium hexafluoride enrichment process

Low enriched uranium with enrichment of 2 to 5% 235U (with some exceptions when using 0.72% in natural composition, for example in Canadian CANDU reactors) is used for nuclear power, in contrast to weapons-grade highly enriched uranium with 235U content of over 20% and usually over 90%. Various methods of isotope separation are used to produce enriched uranium, mainly gas centrifugation and, in the past, the gaseous diffusion method. Most of them work with gaseous UF6, which in turn is produced by fluorination of elemental uranium tetrafluoride (UF4 + F2 → UF6) or uranium oxides (UO2F2 + 2 F2 → UF6 + O2), both highly exothermic.

Since UF6 is the only uranium compound that is gaseous at a relatively low temperature, it plays a key role in the nuclear fuel cycle as a substance suitable for separating 235U and 238U. [19] After obtaining enriched UF6, the remainder (approximately 95% of the total mass) is transformed into depleted UF6 , which consists mainly of 238U, because its 235U content is reduced by perhaps a factor of three, and its 234U content by a factor of six (depending on the degree of depletion). In 2020, nearly two million tons of depleted uranium was accumulated in the world. Most of it is stored in the form of DUHF in special steel tanks. [20]

The methods of handling depleted uranium in different countries depends on their nuclear fuel cycle strategy. The International Atomic Energy Agency (IAEA) recognizes that policy determination is the prerogative of the government (para. VII of the Joint Convention on the Safety of Spent Fuel Management and on the Safety of Radioactive Waste Management). [21] Given the technological capabilities and concepts of the nuclear fuel cycle in each country, with access to separation facilities, DUHF may be considered as a valuable raw material on one hand or low-level radioactive waste on the other. Therefore, there is no unified legal and regulatory status for DUHF in the world. The IAEA expert report ISBN   92-64-195254, 2001 and the joint report of the OECD, NEA and IAEA Management of Depleted Uranium, 2001 recognize DUHF as a valuable raw material. [22] [23]

Accumulated DUHF in 2014 by country [24]
Separation plants, countryAccumulated DUHF

(thousand tons)

Annual increase in

DUHF reserves (thousand tons)

Form of storage

of depleted uranium (DUHF, oxide, metal)

USEC / DOE (USA)70030UF6
ROSATOM (Russia)64015UF6
EURODIF (France)20018UF6, U3O8
BNFL (Great Britain)440UF6
URENCO (Germany, the Netherlands, England)436UF6
JNFL, PNC (Japan)380,7UF6
CNNC (China)301,5UF6
SA NEC (South Africa)30UF6
Others (South America)<1,50-
Total≈ 1700≈ 70UF6, (U3O8)

Applications

As a result of chemical conversion of DUHF, anhydrous hydrogen fluoride and/or its aqueous solution (i.e. hydrofluoric acid) are obtained, which have a certain demand in non-nuclear energy markets, such as the aluminum industry, in production of refrigerants, herbicides, pharmaceuticals, high-octane gasoline, plastics, etc. [25] It is also applied in the reuse of hydrogen fluoride in the production of UF6 via the conversion of U3O8 into uranium tetrafluoride (UF4), before further fluorination into UF6. [26]

Processing

There are multiple directions in the world practice of DUHF reprocessing. Some of them have been tested in a semi-industrial setting, while others have been and are being operated on an industrial scale with an effort to reduce the reserves of uranium tailings and provide the chemical industry with hydrofluoric acid and industrial organofluorine products. [27] [28]

Processing methods of depleted uranium hexafluoride
MethodReactionFinal product
PyrohydrolysisUF6 + H2O → UO2F2 + 4 HF

3 UO2F2 + 3 H2O → U3O8 + 6 HF + ½ O2

Triuranium octoxide and hydrofluoric acid (20 -f 50% HF)
Pyrohydrolysis in a fluidized bed (on UO2 pellets)Uranium dioxide (granular) density up to 6 g/cm3 and hydrofluoric acid (up to 90% HF)
Hydrogen recoveryUF6 + H2 → UF4 + 2 HFUranium tetrafluoride and hydrogen fluoride
Recovery via organic compounds (CHCI)UF6 + CHCI = CCI2 → UF4 + CHCIF - CCI2FUranium tetrafluoride, refrigerants, including ozone-safe (X-122)
Recovery via organic compounds (ССI4)UF6 + CCI4 → UF4 + CF2CI2 + CI2Uranium tetrafluoride and methane-type refrigerants
Plasma-chemical conversionUF6 + 3 H - OH → 1/3 U3O8 + 6 HF + 1/6 O2Triuranium octoxide (density 4.5-4.7 g/cm3) and hydrogen fluoride
Radiation-chemical recovery UF6UF6 + 2 e → UF4 + 2 FUranium tetrafluoride and fluorine.

Depending on nuclear fuel cycle strategy, technological capabilities, international conventions and programs, such as the Sustainable Development Goals (SDG) and the UN Global Compact, each country approaches the issue of the use of accumulated depleted uranium individually. [21] [29] [30] The United States has adopted a number of long-term programs for the safe storage and reprocessing of DUHF stocks prior to their final disposal. [31] [32] [33]

Sustainable development goals

Under the UN SDG, nuclear power plays a significant role not only in providing access to affordable, reliable, sustainable and modern energy (Goal 7), but also in contributing to other goals, including supporting poverty, hunger and water scarcity elimination, economic growth and industry innovation. [34] [35] Several countries, such as the United States, France, Russia, and China, through their leading nuclear power operators, have committed to achieving the Sustainable Development Goals. [36] To achieve these goals, various technologies are being applied both in the reprocessing of spent fuel and in the reprocessing of accumulated DUHF. [37] [38] [39] [40] [41]

Transportation

International policies for transporting radioactive materials are regulated by the IAEA since 1961. [42] [43] These regulations are implemented in the policies of the International Civil Aviation Organization, International Maritime Organization, and regional transport organizations. [44]

Depleted UF6 is transported and stored under standard conditions in solid form and in sealed metal containers with wall thickness of about 1 cm (0.39 in), designed for extreme mechanical and corrosive impacts. [45] For example, the most common "48Y" containers for transportation and storage contain up to 12.5 tons of DUHF in solid form. [46] [47] DUHF is loaded and unloaded from these containers under factory conditions when heated, in liquid form and via special autoclaves. [48]

Dangers

Due to its low radioactivity, the main health hazards of DUHF are connected to its chemical effects on bodily functions. Chemical exposure is a major hazard at facilities associated with the processing of DUHF. Uranium and fluoride compounds such as hydrogen fluoride (HF) are toxic at low levels of chemical exposure. When DUHF comes in contact with air moisture, it reacts to form HF and gaseous uranyl fluoride. HF is a corrosive acid that can be extremely dangerous if inhaled; it is one of the major work hazards in such industries. [20]

In many countries, current occupational exposure limits for soluble uranium compounds are related to a maximum concentration of 3 μg of uranium per gram of kidney tissue. Any effects caused by exposure to these levels on the kidneys are considered minor and temporary. Current practices based on these limits provide adequate protection for workers in the uranium industry. To ensure that these kidney concentrations are not exceeded, legislation limits long-term (8 hours) concentrations of soluble uranium in workplace air to 0.2 mg per cubic meter and short-term (15 minutes) to 0.6 mg per cubic meter [4]

Incidents during transportation

In August 1984, the freighter MS Mont Louis sank in the English Channel with 18 containers of slightly depleted (0.67% 238U) uranium hexafluoride on board, along with enriched and natural UF6. The 30 containers (type 48Y) of UF6 were recovered, as well as 16 of the 22 empty containers (type 30B). Examination of the 30 containers revealed, in one case, a small leak in the shutoff valve. There were 217 samples taken, subjected to 752 different analyses and 146 measurements of dose levels on the containers. There was no evidence of leakage of either radioactive (natural or recycled uranium) or hazardous chemical substances (fluorine or hydrofluoric acid). [49] [50] According to The Washington Post, this incident was not hazardous because the uranium cargo was in its natural state, with an isotope 235U content of 0.72% or less, and only some of it was enriched to 0.9%. [51]

See also

Notes

  1. ↑ This specific activity includes the activity of uranium-234 which is concentrated during the enrichment process, and does not include activity of daughter products.

Related Research Articles

<span class="mw-page-title-main">Uranium</span> Chemical element with atomic number 92 (U)

Uranium is a chemical element; it has symbol U and atomic number 92. It is a silvery-grey metal in the actinide series of the periodic table. A uranium atom has 92 protons and 92 electrons, of which 6 are valence electrons. Uranium radioactively decays, usually by emitting an alpha particle. The half-life of this decay varies between 159,200 and 4.5 billion years for different isotopes, making them useful for dating the age of the Earth. The most common isotopes in natural uranium are uranium-238 and uranium-235. Uranium has the highest atomic weight of the primordially occurring elements. Its density is about 70% higher than that of lead and slightly lower than that of gold or tungsten. It occurs naturally in low concentrations of a few parts per million in soil, rock and water, and is commercially extracted from uranium-bearing minerals such as uraninite.

<span class="mw-page-title-main">Depleted uranium</span> Uranium with lower content of 235U

Depleted uranium is uranium with a lower content of the fissile isotope 235U than natural uranium. Natural uranium contains about 0.72% 235U, while the DU used by the U.S. Department of Defense contains 0.3% 235U or less. The less radioactive and non-fissile 238U constitutes the main component of depleted uranium.

Enriched uranium is a type of uranium in which the percent composition of uranium-235 has been increased through the process of isotope separation. Naturally occurring uranium is composed of three major isotopes: uranium-238, uranium-235, and uranium-234. 235U is the only nuclide existing in nature that is fissile with thermal neutrons.

In physics, natural abundance (NA) refers to the abundance of isotopes of a chemical element as naturally found on a planet. The relative atomic mass of these isotopes is the atomic weight listed for the element in the periodic table. The abundance of an isotope varies from planet to planet, and even from place to place on the Earth, but remains relatively constant in time.

<span class="mw-page-title-main">Nuclear fuel cycle</span> Process of manufacturing and consuming nuclear fuel

The nuclear fuel cycle, also called nuclear fuel chain, is the progression of nuclear fuel through a series of differing stages. It consists of steps in the front end, which are the preparation of the fuel, steps in the service period in which the fuel is used during reactor operation, and steps in the back end, which are necessary to safely manage, contain, and either reprocess or dispose of spent nuclear fuel. If spent fuel is not reprocessed, the fuel cycle is referred to as an open fuel cycle ; if the spent fuel is reprocessed, it is referred to as a closed fuel cycle.

<span class="mw-page-title-main">Nuclear reprocessing</span> Chemical operations that separate fissile material from spent fuel to be recycled as new fuel

Nuclear reprocessing is the chemical separation of fission products and actinides from spent nuclear fuel. Originally, reprocessing was used solely to extract plutonium for producing nuclear weapons. With commercialization of nuclear power, the reprocessed plutonium was recycled back into MOX nuclear fuel for thermal reactors. The reprocessed uranium, also known as the spent fuel material, can in principle also be re-used as fuel, but that is only economical when uranium supply is low and prices are high. Nuclear reprocessing may extend beyond fuel and include the reprocessing of other nuclear reactor material, such as Zircaloy cladding.

<span class="mw-page-title-main">Uranium hexafluoride</span> Chemical compound

Uranium hexafluoride, sometimes called hex, is an inorganic compound with the formula UF6. Uranium hexafluoride is a volatile and toxic white solid that reacts with water, releasing corrosive hydrofluoric acid. The compound reacts mildly with aluminium, forming a thin surface layer of AlF3 that resists any further reaction from the compound. UF6 is used in the process of enriching uranium, which produces fuel for nuclear reactors and nuclear weapons.

<span class="mw-page-title-main">Uranium-238</span> Isotope of uranium

Uranium-238 is the most common isotope of uranium found in nature, with a relative abundance of 99%. Unlike uranium-235, it is non-fissile, which means it cannot sustain a chain reaction in a thermal-neutron reactor. However, it is fissionable by fast neutrons, and is fertile, meaning it can be transmuted to fissile plutonium-239. 238U cannot support a chain reaction because inelastic scattering reduces neutron energy below the range where fast fission of one or more next-generation nuclei is probable. Doppler broadening of 238U's neutron absorption resonances, increasing absorption as fuel temperature increases, is also an essential negative feedback mechanism for reactor control.

<span class="mw-page-title-main">Gas centrifuge</span> Device that performs isotope separation of gases

A gas centrifuge is a device that performs isotope separation of gases. A centrifuge relies on the principles of centrifugal force accelerating molecules so that particles of different masses are physically separated in a gradient along the radius of a rotating container. A prominent use of gas centrifuges is for the separation of uranium-235 (235U) from uranium-238 (238U). The gas centrifuge was developed to replace the gaseous diffusion method of 235U extraction. High degrees of separation of these isotopes relies on using many individual centrifuges arranged in series that achieve successively higher concentrations. This process yields higher concentrations of 235U while using significantly less energy compared to the gaseous diffusion process.

<span class="mw-page-title-main">Gaseous diffusion</span> Old method of enriching uranium

Gaseous diffusion is a technology that was used to produce enriched uranium by forcing gaseous uranium hexafluoride (UF6) through microporous membranes. This produces a slight separation (enrichment factor 1.0043) between the molecules containing uranium-235 (235U) and uranium-238 (238U). By use of a large cascade of many stages, high separations can be achieved. It was the first process to be developed that was capable of producing enriched uranium in industrially useful quantities, but is nowadays considered obsolete, having been superseded by the more-efficient gas centrifuge process (enrichment factor 1.05 to 1.2).

<span class="mw-page-title-main">Atomic vapor laser isotope separation</span>

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<span class="mw-page-title-main">Uranium-234</span> Isotope of uranium

Uranium-234 is an isotope of uranium. In natural uranium and in uranium ore, 234U occurs as an indirect decay product of uranium-238, but it makes up only 0.0055% of the raw uranium because its half-life of just 245,500 years is only about 1/18,000 as long as that of 238U. Thus the ratio of 234
U to 238
U in a natural sample is equivalent to the ratio of their half-lives. The primary path of production of 234U via nuclear decay is as follows: uranium-238 nuclei emit an alpha particle to become thorium-234. Next, with a short half-life, 234Th nuclei emit a beta particle to become protactinium-234 (234Pa), or more likely a nuclear isomer denoted 234mPa. Finally, 234Pa or 234mPa nuclei emit another beta particle to become 234U nuclei.

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<span class="mw-page-title-main">Uranium metallurgy</span>

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Separation of isotopes by laser excitation (SILEX) is a process for enriching uranium to fuel nuclear reactors that may also present a growing nuclear weapons proliferation risk. It is strongly suspected that SILEX utilizes laser condensation repression to excite a vibrational mode of the uranium-235 isotope in uranium hexaflouride (UF6), allowing this lighter molecule to move more rapidly to the outer rim of a gaseous jet and resist condensing compared to the heavier, unexcited 238UF6. This differs greatly from previous methods of laser enrichment explored for their commercial prospects: one using atomic uranium (Atomic Vapor Laser Isotope Separation (AVLIS)) and another molecular method that uses lasers to dissociate a fluorine atom from 235UF6 (Molecular Laser Isotope Separation (MLIS)), allowing the enriched product to precipitate out as a solid.

Uranium-236 (236U) is an isotope of uranium that is neither fissile with thermal neutrons, nor very good fertile material, but is generally considered a nuisance and long-lived radioactive waste. It is found in spent nuclear fuel and in the reprocessed uranium made from spent nuclear fuel.

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  47. ↑ Uranium hexafluoride: A manual of good handling practices. Revision 7 (Technical report). Bethesda, MA: U.S. Enrichment Corp. 1995. OSTI   205924 .
  48. ↑ Affordable Cleanup?: Opportunities for Cost Reduction in the Decontamination and Decommissioning of the Nation's Uranium Enrichment Facilities. National Academy Press. 1996. p. 157. doi: 10.17226/5114 . ISBN   978-0-309-05438-6.
  49. ↑ Bernard Augustin. "The sinking of the Mont-Louis and nuclear safety" (PDF). iaea.org. pp. 28–31.
  50. ↑ "INIS Repository Search - Single Result". inis.iaea.org. Retrieved 2020-12-26.
  51. ↑ The Washington Post. "A Cargo of Uranium". washingtonpost.com.
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