 Plutonium-238 oxide pellet glowing from its decay heat | |
| General | |
|---|---|
| Symbol | 238Pu |
| Names | plutonium-238 |
| Protons(Z) | 94 |
| Neutrons(N) | 144 |
| Nuclide data | |
| Half-life(t1/2) | 87.7 years[1] |
| Isotope mass | 238.049553[2]Da |
| Spin | 0 |
| Parent isotopes | 242Cm (α) 238Np (β−) 238Am (β+) |
| Decay products | 234U |
| Decay modes | |
| Decay mode | Decay energy (MeV) |
| Alpha decay | 5.593[3] |
| Isotopes of plutonium Complete table of nuclides | |
Plutonium-238 (238
Pu orPu-238) is aradioactiveisotope of plutonium that has ahalf-life of 87.7 years.
Plutonium-238 is a very powerfulalpha emitter; as alpha particles are easily blocked, this makes the plutonium-238 isotope suitable for usage inradioisotope thermoelectric generators (RTGs) andradioisotope heater units. The density of plutonium-238 at room temperature is about 19.8 g/cc.[4] The material will generate about 0.57 watts per gram of238Pu.[5]
The bare spherecritical mass of metallic plutonium-238 is not precisely known, but its calculated range is between 9.04 and 10.07 kg (19.9 and 22.2 lb).[6]
Plutonium-238 was the firstisotope of plutonium to be discovered. It was synthesized byGlenn Seaborg and his associates in December 1940 by bombardinguranium-238 withdeuterons, creatingneptunium-238.
238
92U +2
1H →238
93Np + 2n
The neptunium isotope then undergoesβ− decay to plutonium-238 with a half-life of 2.099 days.[7]
Plutonium-238 naturally decays touranium-234 and then continues, after a long period of time, along theradium series tolead-206. Historically, most plutonium-238 has been produced bySavannah River in their weapons reactor, by irradiating neptunium-237 (half life2.144 Ma) with neutrons.[8]
237
93Np +n →238
93Np
Neptunium-237 is a by-product of the production ofplutonium-239 weapons-grade material, and when the site was shut down in 1988,238Pu was mixed with about 16%239Pu.[9]
Plutonium was first synthesized in 1940 and isolated in 1941 by chemists at the University of California, Berkeley.[10][11]
TheManhattan Project began shortly after the discovery, with most early research (pre-1944) carried out using small samples manufactured using the largecyclotrons at the BerkeleyRad Lab andWashington University in St. Louis.[12]
Much of the difficulty encountered during the Manhattan Project regarded the production and testing of nuclear fuel. Bothuranium and plutonium were eventually determined to befissile, but in each case they had to be purified to select for the isotopes suitable for anatomic bomb.[13]
WithWorld War II underway, the research teams were pressed for time. Micrograms of plutonium were made by cyclotrons in 1942 and 1943. In late 1943Robert Oppenheimer is quoted as saying "there's only a twentieth of a milligram in existence."[12]
By his request, the Rad Lab at Berkeley made available 1.2 mg of plutonium by the end of October 1943, most of which was taken to Los Alamos for theoretical work there.[12]
The world's second reactor, theX-10 Graphite Reactor built at a secret site atOak Ridge, would be fully operational in 1944. In November 1943, shortly after its initial start-up, it was able to produce a minuscule 500 mg. However, this plutonium was mixed with large amounts of uranium fuel and destined for the nearby chemical processing pilot plant forisotopic separation (enrichment). Gram amounts of plutonium would not be available until early 1944.[14]
Industrial-scale production of plutonium only began in March 1945 when theB Reactor at theHanford Site began operation.[13]
While samples of plutonium were available in small quantities and being handled by researchers, no one knew what health effects this might have.[13]
Plutonium handling mishaps occurred in 1944, causing alarm in the Manhattan Project leadership as contamination inside and outside the laboratories was becoming an issue.[13] In August 1944, chemistDonald Mastick was sprayed in the face with a solution ofplutonium chloride, causing him to accidentally swallow some.[13][15] Nose swipes taken of plutonium researchers indicated that plutonium was being breathed in.[13][16] Lead Manhattan Project chemistGlenn Seaborg, discoverer of manytransuranium elements including plutonium, urged that a safety program be developed for plutonium research. In a memo to Robert Stone at the ChicagoMet Lab, Seaborg wrote "that a program to trace the course of plutonium in the body be initiated as soon as possible ... [with] the very highest priority."[17] This memo was dated January 5, 1944, prior to many of the contamination events of 1944 in Building D where Mastick worked.[12] Seaborg later claimed that he did not at all intend to imply human experimentation in this memo, nor did he learn of its use in humans until far later due to the compartmentalization ofclassified information.[12]
With bomb-grade enrichedplutonium-239 destined for critical research and for atomic weapon production, plutonium-238 was used in early medical experiments as it is unusable as atomic weapon fuel. However,238Pu is far more dangerous than239Pu due to its short half-life and being a strong alpha-emitter. It was soon found that plutonium was being excreted at a very slow rate, accumulating in test subjects involved in earlyhuman experimentation. This led to severe health consequences for the patients involved.
From April 10, 1945, to July 18, 1947, eighteen people were injected with plutonium as part of the Manhattan Project. Doses administered ranged from 0.095 to 5.9microcuries (μCi).[13]
Albert Stevens, after a (mistaken) terminal cancer diagnosis which seemed to include many organs, was injected in 1945 with plutonium without hisinformed consent. He was referred to as patient CAL-1 and the plutonium consisted of 3.5 μCi238Pu and 0.046 μCi239Pu, giving him an initial body burden of 3.546 μCi (131kBq) total activity.[18][13] The fact that he had the highly radioactive plutonium-238 (produced in the 60-inchcyclotron at the Crocker Laboratory by deuteron bombardment of natural uranium)[18] contributed heavily to his long-term dose. Had all of the plutonium given to Stevens been the long-lived239Pu as used in similar experiments of the time, Stevens's lifetime dose would have been significantly smaller. The shorthalf-life of 87.7 years of238Pu means that a large amount of it decayed during its time inside his body, especially when compared to the 24,100 year half-life of239Pu.
After his initial "cancer" surgery removed many non-cancerous "tumors", Stevens survived for about 20 years after his experimental dose of plutonium before succumbing to heart disease; he had received the highest known accumulated radiation dose of any human patient.[12] Modern calculations of hislifetime absorbed dose give a significant 64 Sv (6400 rem) total.[12]
The first application of238Pu was its use innuclear weapon components made atMound Laboratories for Lawrence Radiation Laboratory (nowLawrence Livermore National Laboratory). Mound was chosen for this work because of its experience in producing thepolonium-210-fueledUrchin initiator and its work with several heavy elements in a Reactor Fuels program. Two Mound scientists spent 1959 at Lawrence in joint development while the Special Metallurgical Building was constructed at Mound to house the project. Meanwhile, the first sample of238Pu came to Mound in 1959.[19]
The weapons project called for the production of about 1 kg/year of238Pu over a 3-year period. However, the238Pu component[clarification needed] could not be produced to the specifications despite a 2-year effort beginning at Mound in mid-1961. A maximum effort was undertaken with 3 shifts a day, 6 days a week, and ramp-up ofSavannah River's238Pu production over the next three years to about 20 kg/year. A loosening of the specifications resulted in productivity of about 3%,[clarification needed] and production finally began in 1964.[citation needed]
Beginning on January 1, 1957, Mound Laboratories RTG inventors Jordan & Birden were working on an Army Signal Corps contract (R-65-8- 998 11-SC-03-91) to conduct research on radioactive materials andthermocouples suitable for the direct conversion of heat to electrical energy using polonium-210 as the heat source.
In 1961, Capt. R. T. Carpenter had chosen238Pu as the fuel for the first RTG (radioisotope thermoelectric generator) to be launched into space as auxiliary power for theTransit IV Navy navigational satellite. By January 21, 1963, the decision had yet to be made as to what isotope would be used to fuel the large RTGs for NASA programs.[20]
Early in 1964, Mound Laboratories scientists developed a different method of fabricating the weapon component that resulted in a production efficiency of around 98%.[21] This made available the excess Savannah River238Pu production for Space Electric Power use just in time to meet the needs of theSNAP-27 RTG on the Moon, the Pioneer spacecraft, theViking Mars landers, moreTransit Navy navigation satellites (precursor to today'sGPS) and twoVoyager spacecraft, for which all of the238Pu heat sources were fabricated at Mound Laboratories.[22]
The radioisotope heater units were used in space exploration beginning with the Apollo Radioisotope Heaters (ALRH) warming theSeismic Experiment placed on the Moon by theApollo 11 mission and on severalMoon andMars rovers, to the 129 LWRHUs warming the experiments on theGalileo spacecraft.[23]
An addition to the Special Metallurgical building weapon component production facility was completed at the end of 1964 for238Pu heat source fuel fabrication. A temporary fuel production facility was also installed in the Research Building in 1969 forTransit fuel fabrication. With completion of the weapons component project, the Special Metallurgical Building, nicknamed "Snake Mountain" because of the difficulties encountered in handling large quantities of238Pu, ceased operations on June 30, 1968, with238Pu operations taken over by the new Plutonium Processing Building,[where?] especially designed and constructed for handling large quantities of238Pu. Plutonium-238 is given the highest relative hazard number (152) of all 256 radionuclides evaluated by Karl Z. Morgan et al. in 1963.[24]
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In the United States, when plutonium-238 became available for non-military uses, numerous applications were proposed and tested, including thecardiac pacemaker program that began on June 1, 1966, in conjunction with NUMEC.[25] The last of these units was implanted in 1988, as lithium-powered pacemakers, which had an expected lifespan of 10 or more years without the disadvantages of radiation concerns and regulatory hurdles, made these units obsolete.[26]
As of 2007[update], there were nine living people with nuclear-powered pacemakers in the United States, out of an original 139 recipients.[27] When these individuals die, the pacemaker is supposed to be removed and shipped to Los Alamos where the plutonium will be recovered.[28]
In a letter to theNew England Journal of Medicine discussing a woman who received a Numec NU-5 decades ago that is continuously operating, despite an original $5,000 price tag equivalent to $23,000 in 2007 dollars, the follow-up costs have been about $19,000 compared with $55,000 for a battery-powered pacemaker.[27]
Another nuclear powered pacemaker was the Medtronics “Laurens-Alcatel Model 9000”.[29] Approximately 1600 nuclear-powered cardiac pacemakers and/or battery assemblies have been located across the United States, and are eligible for recovery by the Off-Site Source Recovery Project (OSRP) Team at Los Alamos National Laboratory (LANL).[30]
Reactor-grade plutonium fromspent nuclear fuel contains variousisotopes of plutonium.238Pu makes up only one or two percent, but it may be responsible for much of the short-termdecay heat because of its shorthalf-life relative to other plutonium isotopes. Reactor-grade plutonium is not useful for producing238Pu forRTGs because difficultisotopic separation would be needed.
Pure plutonium-238 is prepared byneutron irradiation ofneptunium-237,[31] one of theminor actinides that can be recovered fromspent nuclear fuel duringreprocessing, or by the neutron irradiation ofamericium in a reactor.[32] The targets are purified chemically, including dissolution innitric acid to extract the plutonium-238. A 100 kg sample oflight water reactor fuel that has been irradiated for three years contains only about 700 grams (0.7% by weight) of neptunium-237, which must be extracted and purified.
In the US, theDepartment of Energy's Space and Defense Power Systems Initiative of theOffice of Nuclear Energy processes238Pu, maintains its storage, and develops, produces, transports and manages safety of radioisotope power and heating units for bothspace exploration andnational security spacecraft.[33]As of March 2015, a total of 35 kilograms (77 pounds) of238Pu was available for civil space uses. Out of the inventory, 17 kg (37 lb) remained in a condition meeting NASA specifications for power delivery. Some of this pool of238Pu was used in amulti-mission radioisotope thermoelectric generator (MMRTG) for the2020 Mars Rover mission and two additional MMRTGs for a notional 2024 NASA mission. 21 kg (46 lb) would remain after that, including approximately 4 kg (8.8 lb) just barely meeting the NASA specification.Since isotope content in the material is lost over time to radioactive decay while in storage, this stock could be brought up to NASA specifications by blending it with a smaller amount of freshly produced238Pu with a higher content of the isotope, and therefore energy density.[34]
The United States stopped producing bulk238Pu with the closure of theSavannah River Site reactors in 1988.[35][36][37] Since 1993, all of the238Pu used in American spacecraft has been purchased from Russia. From 1992 to 1994, 10 kilograms were purchased by theUS Department of Energy from Russia'sMayak Production Association. Via agreement withMinatom, the US must use plutonium for uncrewed NASA missions, and Russia must use the currency for environmental and social investment in theChelyabinsk region, affected by long-termradioactive contamination such as theKyshtym disaster.[38] In total, 16.5 kilograms (36 lb) have been purchased, but Russia is no longer producing238Pu, and their own supply is reportedly running low.[39][40]
In February 2013, a small amount of238Pu was successfully produced by Oak Ridge'sHigh Flux Isotope Reactor,[41] and on December 22, 2015, they reported the production of 50 grams (1.8 ounces) of238Pu.[42][43]
In March 2017,Ontario Power Generation (OPG) and its venture arm, Canadian Nuclear Partners, announced plans to produce238Pu as a second source for NASA. Rods containingneptunium-237[44] will be fabricated byPacific Northwest National Laboratory (PNNL) in Washington State and shipped to OPG'sDarlington Nuclear Generating Station inClarington, Ontario, Canada where they will be irradiated with neutrons inside the reactor's core to produce238Pu.[45][46]
In January 2019, it was reported that some automated aspects of its production were implemented at Oak Ridge National Laboratory in Tennessee, that are expected to triple the number of plutonium pellets produced each week.[47] The production rate is now expected to increase from 80 pellets per week to about 275 pellets per week, for a total production of about 400 grams per year.[47] The goal now is to optimize and scale-up the processes in order to produce an average of 1.5 kg (3.3 lb) per year by 2025.[48][46]
In 2023, theDoE delivered 0.5 kg of Pu-238 for NASA missions and expected to produce 1.5 kg per year of plutonium oxide by 2026.[49]
The main application of238Pu is as the heat source inradioisotope thermoelectric generators (RTGs). The RTG was invented in 1954 by Mound scientists Ken Jordan and John Birden, who were inducted into the National Inventors Hall of Fame in 2013.[50] They immediately produced a working prototype using a210Po heat source, and on January 1, 1957, entered into an Army Signal Corps contract (R-65-8- 998 11-SC-03-91) to conduct research on radioactive materials and thermocouples suitable for the direct conversion of heat to electrical energy usingpolonium-210 as the heat source.
In 1966, a study reported bySAE International described the potential for the use of plutonium-238 in radioisotope power subsystems for applications in space. This study focused on employing power conversions through theRankine cycle,Brayton cycle,thermoelectric conversion andthermionic conversion with plutonium-238 as the primary heating element. The heat supplied by the plutonium-238 heating element was consistent between the 400 °C and 1000 °C regime but future technology could reach an upper limit of 2000 °C, further increasing the efficiency of the power systems. The Rankine cycle study reported an efficiency between 15 and 19% with inletturbine temperatures of 730 °C, whereas the Brayton cycle offered efficiency greater than 20% with an inlet temperature of 840 °C.Thermoelectric converters offered low efficiency (3-5%) but high reliability.Thermionic conversion could provide similar efficiencies to the Brayton cycle if proper conditions reached.[51]
RTG technology was first developed byLos Alamos National Laboratory during the 1960s and 1970s to provide radioisotope thermoelectric generator power forcardiac pacemakers. Of the 250 plutonium-powered pacemakersMedtronic manufactured, twenty-two were still in service more than twenty-five years later, a feat that no battery-powered pacemaker could achieve.[52]
This same RTG power technology has been used in spacecraft such asPioneer 10 and11,Voyager 1 and2,Cassini–Huygens andNew Horizons, and in other devices, such as theMars Science Laboratory andMars 2020Perseverance Rover, for long-term nuclear power generation.[53]
{{cite book}}:ISBN / Date incompatibility (help)| Lighter: plutonium-237 | Plutonium-238 is an isotope ofplutonium | Heavier: plutonium-239 |
| Decay product of: curium-242(α) americium-238(β+) neptunium-238(β−) uranium-238(β−β−) | Decay chain of plutonium-238 | Decays to: uranium-234(α) |