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Nuclear Waste
Nuclear Waste
Encyclopedia of Energy, Volume 4. r 2004 Elsevier Inc. All rights reserved. 449
450 Nuclear Waste
number A, and nuclear energy distinct from any other U-235 (0.71% by weight) and U-238 (99.28% by
species of atom. weight). Only U-235 is fissile, meaning that it readily
radionuclide A radioactive nuclide. undergoes fission by the absorption of slow neutrons.
radiotoxicity A measure of the potential of a radioactive The fission of U-235 can be represented by
substance to cause harm to living tissue by radiation
after introduction into the body. n þ235 U-fission fragments þ 2:43n:
reprocessing The separation of spent nuclear fuel into
useful materials (especially uranium and plutonium) A fission reaction produces two (or more) fission
and wastes. fragments or products and additional neutrons (2.43
solvent extraction A process for removing chemical solutes neutrons on average); the latter can initiate further
from a liquid solution using a second immiscible liquid fission reactions. Each fission reaction releases
phase. approximately 200 MeV (million electronvolts) of
spent nuclear fuel Fuel after it has been used in a nuclear energy, predominantly as the kinetic energy of the
reactor, containing fission products, plutonium, and fission fragments. In contrast, the chemical combus-
unreacted uranium. tion of a hydrocarbon fuel typically releases less than
transuranic element An element having an atomic number 7 eV per molecule of CO2 formed.
Z greater than 92.
The more abundant uranium isotope U-238 is
tuff Rock formed from consolidated volcanic ash; welded
tuff results when ash particles are fused together by heat
not fissile. However, U-238 is fertile, meaning that
and pressure. it can capture neutrons and be converted to
vitrification The process of converting or incorporating plutonium-239:
nuclear wastes into a glass for permanent disposal. n þ238 U-239 Pu:
yellowcake The solid product of uranium milling, nomin-
ally U3O8 but actually consisting of mixed uranium Plutonium-239 is fissile:
oxides, hydrides, and impurities.
n þ239 Pu-fission fragments þ 2:88n:
Depleted
3. Enrichment 7. Reprocessing
uranium
m
aniu
Uranium hexafluoride Ur High-level waste
1. NUCLEAR FISSION
2. Conversion 8. Immobilization
All commercial nuclear power plants rely on the
Yellowcake Immobilized waste
fission of uranium and, to a lesser extent, plutonium.
Uranium
(An alternative cycle, based on thorium, has been mill 1. Mining and milling 9. Final disposal
explored but never commercialized.) Naturally oc- tailings
curring uranium consists of two major isotopes: FIGURE 1 Nuclear fuel cycle based on uranium.
Nuclear Waste 451
2.1 Mining and Milling mately 75 metric tons (165,000 pounds) of enriched
uranium oxide fuel. Approximately 25 metric tons
Uranium is excavated from open-pit or deep-shaft
(55,000 pounds) of fresh fuel is required each year.
mines using conventional mining techniques (step 1 in
Thus, each fuel assembly spends about 3 years in the
the fuel cycle). The ore is crushed and the uranium is
reactor core. The heat from the fission reactions is
leached out using sulfuric acid or sodium carbonate
used to generate steam for running power turbines.
and bicarbonate. The uranium is recovered from the
Most of the power output comes from the fission of
liquid using processes such as ion exchange, solvent U-235. However, some U-238 is transformed into Pu-
extraction, precipitation, and drying. The product is
239, the fission of which provides about a third of
yellowcake, a solid consisting of U3O8 and various
the reactor’s energy output.
other oxides, hydroxides, and impurities.
geological repository in stable crystalline rock, salt tend to have neutron-rich nuclei with mass numbers
deposits, or clay. from approximately 70 to 160, with peak production
occurring near mass numbers 95 and 135. Most
fission products are beta or beta/gamma emitters.
3. RADIONUCLIDES IN Heavy nuclei. Nuclei having mass numbers
NUCLEAR WASTE between 232 and 246 are used as fuels for nuclear
fission or are produced by neutron capture in fission
reactions. Most of these are long-lived alpha emitters.
More than 2500 nuclides have been discovered or
created. Most of these are too short-lived to be of Table I lists some radionuclides of concern in
practical interest. The Index of Radioisotopes, nuclear wastes. These radionuclides are also dis-
published by the U.S. Nuclear Regulatory Commis- cussed in detail in what follows.
sion (NRC), lists some 770 isotopes. Those of
concern in radioactive wastes generally fall into one 3.1 Americium
of three categories:
Americium (Am, atomic number 95) is an artificial
Activation products. Substances used as cool- actinide. Its most important isotope is americium-
ants, moderators, and reactor structures can become 241 (half-life 432.7 years), which is produced by the
radioactive by absorbing neutrons. These are usually beta-decay of plutonium-241. Americium-241 is
light- or medium-mass nuclides. used commercially in applications such as smoke
Medium-mass fission products. The fission of detectors, thickness gauges, and fluid level gauges.
uranium produces more than 200 different radio- Although americium-241 has very high radiotoxicity,
nuclides, covering about a third of the periodic table it is not very mobile in the environment. It decays by
from copper to the lanthanides. Fission fragments alpha emission to neptunium-237.
TABLE I
Some Radionuclides in Nuclear Wastes
(half-life 3.76 105 years). All of these isotopes have 3.14 Technetium
very high radiotoxicity.
The first artificially produced element, technetium
(Tc, atomic number 43) occurs in nature only in
3.10 Radium minute amounts. At least 34 isotopes have been
produced, having atomic masses ranging from 85 to
Radium (Ra, atomic number 88) is a naturally
118; of these, the beta-emitter technetium-99 (half-
occurring radioactive element. Radium-228 (half-life
5.76 years) is a decay product of thorium; radium- life 2.13 105 years) is of special concern because it
is produced in fission reactors, both as a fission
226 (half-life 1600 years) is a decay product of
fragment and as an activation product. Like iodine,
uranium. Radium-226 and its daughters (including
technetium is absorbed by the thyroid. The radio-
radon-222) are the major sources of radioactivity in
toxicity of technetium is relatively low.
uranium mine tailings. Chemically, radium is an
alkaline earth metal like calcium and tends to
concentrate in the bone. The radiotoxicity of radium 3.15 Thorium
is very high.
Thorium (Th, atomic number 90) is a naturally
occurring radioactive element, several times more
3.11 Radon abundant than uranium, which has been considered
as the basis for an alternative fuel cycle. The most
Radon (Rn, atomic number 86) is a radioactive noble
important natural isotope is thorium-232 (half-life
gas produced by the decay of radium. The two most
14.0 10 years), which is weakly radioactive, decay-
important isotopes are the alpha-emitters radon-220
ing by alpha and gamma emission to radium-228.
(half-life 54.6 s) and radon-222 (half-life 3.82 days).
The radiotoxicity of thorium-232 is relatively low.
Being a gas, radon is highly mobile; in some areas,
radon is a concern because it can accumulate in Another isotope, thorium-230 (half-life 75,400
years) is produced naturally by the decay of
buildings. Both radon-220 and radon-222 are
uranium-234. The radiotoxicity of thorium-230 is
moderately radiotoxic.
very high. A third isotope, thorium-228 (half-life 1.9
years) also has very high radiotoxicity.
3.12 Ruthenium
Ruthenium (Ru, atomic number 44) belongs to the 3.16 Uranium
platinum family of metals. It has seven stable natural
isotopes. The most important radioactive isotope is Uranium (U, atomic number 92) is the heaviest
element found in appreciable amounts in nature,
ruthenium-106 (half-life 372.2 days), a fission
making up 2 to 4 grams per metric ton of the earth’s
product that decays by low-energy beta emission to
crust. Natural uranium consists of 99.283% by
rhodium-106 (a high-energy beta/gamma emitter
weight uranium-238 (half-life 4.468 109 years),
with half-life of 30 s). Ruthenium-106 has high
0.711% uranium-235 (half-life 7.04 108 years),
radiotoxicity.
and 0.005% uranium-234 (half-life 245,000 years).
All three isotopes are alpha-emitters. Natural ura-
3.13 Strontium nium has relatively low radiotoxicity.
Strontium (Sr, atomic number 38) is an alkaline earth
metal lying below calcium in the periodic table. Four
stable isotopes are found in nature, and 16 radio- 4. CLASSIFICATION OF
active isotopes have been produced artificially. Most
RADIOACTIVE WASTE
of the radioactive isotopes of strontium are short-
lived and of little interest. The exception is stron-
There is no generally accepted classification scheme
tium-90 (half-life 29.1 years), a beta-emitter that is
for radioactive wastes. The following categories are
produced as a fission fragment. Much of the radio-
commonly defined in the United States:
activity of SNF results from strontium-90. Because
its chemical properties resemble those of calcium, Uranium mill tailings (UMTs) are the residues
strontium-90 tends to concentrate in the bones. It is from the mining and milling of uranium ores. Most
highly radiotoxic, decaying into yttrium-90 (itself an uranium ores in the United States contain uranium at
energetic beta-emitter of moderate radiotoxicity). a concentration of approximately 0.2% (2000 ppm)
Nuclear Waste 455
by weight. Consequently, the production of 1 kg of Under the foregoing classification scheme, com-
uranium metal requires the excavation of 500 kg (or monly followed in the United States, wastes are
more) of ore. Milling creates additional solid and categorized according to their source as well as their
liquid wastes. Tailings generally contain relatively radioactivity. However, other countries tend to
low concentrations of radioactive materials; how- categorize wastes according to their radioactivity
ever, because of the high volumes of tailings, their alone. For example, in the United Kingdom, solid
overall radioactivity can be high. The principal wastes are classified as high-, intermediate-, low-, or
radionuclides of concern in UMTs are radium-226 very low-level wastes as follows:
(half-life 1600 years) and its daughter radon-222
Very low-level waste (VLLW) can safely be
(half-life 3.8 days).
discarded as ordinary refuse. To qualify, bulk waste
Depleted uranium, the major by-product from
must contain less than 400 kBq of beta/gamma
the enrichment process, is uranium containing
activity per 0.1 m3 of material; individual items
less than 0.71% uranium-235. Depleted ura-
must contain less than 40 kBq of beta/gamma
nium currently has few civilian uses but could
activity.
eventually be converted to fissile plutonium in
Low-level waste (LLW) has higher levels of
breeder reactors. The U.S. Department of Energy
radioactivity than can be safely handled as ordinary
(DOE) stores approximately 730,000 metric tons
refuse but not exceeding 4 GBq per metric ton of
of depleted uranium, most of it as uranium hexa-
alpha radiation or 12 GBq per metric ton of beta/
fluoride.
gamma radiation.
Low-level waste (LLW) has relatively low levels
Intermediate-level waste (ILW) has higher radio-
of radioactivity and contains little or no transuranic
activity levels than does LLW but not so high that
radioisotopes (i.e., radionuclides beyond uranium in
heating becomes a concern.
the periodic table). LLW may be further divided into
High-level waste (HLW) has such high levels of
classes A, B, and C, with A being the least hazardous
radioactivity that appreciable thermal heating oc-
and C being the most hazardous. (Some LLW is
curs. Consequently, storage and processing facilities
classified as ‘‘greater than C.’’) Mixed low-level
have to be designed to contain the radiation and
waste (MLLW) contains both low-level radioactive
dissipate the generated heat.
and chemically hazardous substances. Although not
shown in Fig. 1, LLW is generated at every step of
the nuclear fuel cycle and may include used
protective clothing, rags, paper, tools, filter elements, 5. DISPOSAL OF
and so on. LOW-LEVEL WASTE
Spent nuclear fuel (SNF) is the irradiated fuel
discharged from nuclear reactors. It contains fission LLW accounts for approximately 90% of the total
products, plutonium, and unreacted uranium and is volume of all wastes produced in the nuclear fuel cycle
both thermally hot and highly radioactive. but only 1% of the total radioactivity. Various
Transuranic waste (TRUW) contains alpha-emit- methods have been adopted for disposing of LLW,
ting radionuclides having atomic numbers greater depending on the type of waste and its levels of
than 92. To qualify as TRUW under U.S. law, the radioactivity. For example, the NRC requires that
radionuclides must possess half-lives greater than 20 Class A and B wastes be contained for at least 100
years and be present in concentrations greater than years, and Class C waste must be contained for 500
100 nCi/g. Although their radioactivity is relatively years. Combinations of natural and engineered bar-
low, the long lives of the radioisotopes require riers are used to prevent radioactivity from escaping to
long-term storage. Virtually all of the TRUW in the the environment. A major goal is to prevent the
United States is the by-product of nuclear weapons intrusion of ground water and surface water.
production.
High-level waste (HLW) includes the residues
5.1 Shallow Land Burial
resulting from the reprocessing of spent reactor fuel
and the production of nuclear weapons. HLW The cheapest way to dispose of LLW is to bury it in
contains highly radioactive fission products and shallow trenches dug in stable soil (Fig. 2). A typical
small amounts of plutonium isotopes. SNF may be disposal trench may be 6 to 10 m deep, 30 m wide,
considered as HLW in countries that do not reprocess and 100 to 300 m long. In some cases, the trench may
fuel. be lined with a layer of clay, polymer, or concrete.
456 Nuclear Waste
Topsoil Topsoil
Clay cap Clay cap
Backfill Backfill
Waste packages
French drain Drainage layer
Waste packages Vault
French drain Drainage layer
FIGURE 4 Belowground vault disposal.
FIGURE 2 Shallow land burial for LLW.
Drainage layer
Drain Impermeable layer
Waste packages
buried in trenches. The canisters serve as an
French drain Drainage layer
additional barrier against the release of radioactivity.
Concrete canister
structure resembling a large warehouse. The princi- After the waste containers have been stacked in the
pal advantage of an AGV is that it allows easy shaft, it is backfilled with sand or clay and capped
recovery of wastes for further processing or reuse. Its with concrete. Shaft disposal of LLWs has been used
principal disadvantage is that the structure is not at a number of sites in the United States and Canada.
protected by earth from the effects of weather,
intrusions, or accidents. Consequently, an AGV is
often considered more for temporary storage than for 5.7 Deep Geological Disposal
permanent disposal. AGVs have been used at the Some countries have chosen to dispose of LLW and
West Valley Demonstration Project in New York and ILW in deep geological repositories similar to those
at the Point Lepreu and Bruce sites in Canada. planned for HLW. These repositories are to be
located in stable geological media such as igneous
5.5 Earth-Mounded Concrete Bunker rock, salt, or clay.
TABLE II
National Policies on Reprocessing of Spent Nuclear Fuel
Canada, Finland, the United States) do not reprocess. to escape containment. Seabed disposal is still
Still other countries (e.g., Czech Republic, South considered a viable option for the future. However,
Korea, Taiwan) have deferred the decision on an international agreement, the 1993 London Con-
whether to reprocess, relying on storage of SNF for vention, banned the disposal of all radioactive wastes
the near term. at sea for 25 years, after which such disposal
methods may be reconsidered every 25 years.
TABLE III
Plans for High-Level Waste Repositories
The U.S. Atomic Energy Commission (AEC) was nominate five sites for study as possible SNF/HLW
established in 1946 and given the responsibility for repositories. Based on these initial studies, the
both civilian and military nuclear programs. Initially, secretary was to recommend (by January 1, 1985)
waste management was given lower priority than the three of the five sites for intensive study. Finally,
development of nuclear weapons and (later) a one site was to be recommended by March 31, 1987.
nuclear power industry. It was widely expected that The goal was to have the first repository in operation
plants would be constructed to reprocess SNF. by 1998.
Uranium and plutonium would be reused; reproces- The Low-Level Radioactive Waste Policy
sing wastes would be solidified and transferred to a Amendments Act (LLRWPAA) of 1985 was crafted
permanent repository for disposal. to address difficulties arising out of the Low-Level
The National Academy of Sciences recommended Waste Policy Act of 1980. The formation of state
in 1957, and again in 1970, that a federal waste compacts and the development of disposal facilities
repository be built in a stable bedded salt deposit. had taken longer than was expected. The LLRWPAA
Accordingly, in 1970, the AEC investigated salt beds kept open the three existing commercial disposal
near Lyons, Kansas, as a possible site for a repository. sites and set regulations for the disposal of LLW.
However, the Lyons site was rejected in 1972 because The Nuclear Waste Policy Amendments Act of
of concerns about its geology and hydrology as well 1987 specified that Yucca Mountain be the sole site
as the large number of boreholes left by previous oil for study as an HLW repository instead of having
and gas drilling in the area. In 1974, the AEC began three site studies proceeding in parallel. The amend-
exploring salt beds in southeastern New Mexico. The ment also canceled the requirement from the NWPA
next year, a site for the WIPP was selected. of 1982 that a second repository be created. The
In 1974, the AEC was abolished by Congress, and selection of Yucca Mountain was a political decision,
its responsibilities were transferred to two new not a scientific or technical one; local opposition to
agencies. The Energy Research and Development other sites made them less attractive politically.
Administration (ERDA) was created to develop and The Waste Isolation Pilot Plant Land With-
promote nuclear power, and the NRC was created to drawal Act of 1992 transferred control of the WIPP
regulate civilian nuclear programs. In 1976, the U.S. site from the Department of Interior to the DOE. The
Environmental Protection Agency (EPA) was given act also gave the EPA responsibility for ensuring
the responsibility of setting radiation protection compliance with environmental regulations.
standards for nuclear wastes. The next year, the The Energy Policy Act of 1992 was a large and
ERDA was replaced by a new cabinet-level agency, comprehensive piece of legislation covering a broad
the DOE. The new department was also given range of energy policy issues, including energy
responsibility for nuclear weapons programs. efficiency and conservation, integrated resource
Given these organizational changes, it is perhaps planning, alternative fuels, and competitive restruc-
not surprising that the executive branch of the turing of wholesale electricity markets. The act
federal government made little progress in formulat- required that the EPA set standards for the Yucca
ing a coherent policy for nuclear waste management Mountain repository based on recommendations by
during the 1970s. Congress has repeatedly stepped in the National Academy of Sciences. The NRC was to
and formulated policies for waste disposal. Some of assume long-term responsibility for the repository.
the major pieces of legislation include the following:
8.2 Low-Level Waste Repositories
The Low-Level Radioactive Waste Policy Act of
1980 requires each state to be responsible for Six commercial LLW disposal sites have been created
disposing of LLW generated within its borders, either in the United States: Barnwell, North Carolina;
by providing a suitable disposal site or by entering Beatty, Nevada; Richland, Washington; Maxey Flats,
into compacts with other states to develop a shared Kentucky; Sheffield, Illinois; and West Valley, New
site. The disposal sites were to be in operation by York. All of these sites have used some form of SLB.
1986. Because of leaks, the latter three sites have been
The Nuclear Waste Policy Act (NWPA) of 1982 closed.
created the Office of Civilian Radioactive Waste Low-level military wastes have been stored at a
Management in the DOE and gave it the responsi- number of sites around the country, including
bility for developing a system to manage SNF and Amarillo, Texas; Hanford, Washington; the Idaho
HLW. The act also directed the secretary of energy to National Engineering and Environmental Laboratory;
Nuclear Waste 461
Los Alamos, New Mexico; Paducah, Kentucky; and 120 km (75 miles) northwest of Las Vegas. The repo-
Savannah River, South Carolina. sitory is intended for the permanent disposal of SNF
and HLW from both civilian and defense sources.
As planned, the Yucca Mountain repository will
8.3 Waste Isolation Pilot Plant
hold SNF that is currently kept in 131 temporary
The WIPP is an underground waste repository storage facilities in the United States. By 2002, these
located in bedded salt formations in southeastern sites contained some 45,000 metric tons of SNF from
New Mexico, approximately 40 km (25 miles) east of commercial reactors and 2500 metric tons from
Carlsbad. The WIPP repository was created for the defense reactors. Another 380,000 m3 of liquid HLW
permanent disposal of TRUW resulting from nuclear from nuclear weapons production was stored at sites
weapons production. It is the first deep geological operated by the DOE; this waste is to be stabilized in
repository designed specifically for long-term dis- the form of borosilicate glass.
posal of nuclear waste. Yucca Mountain is composed of tuff, a material
The waste destined for the WIPP site consists of a formed from volcanic ash and dust. Some of the tuff
variety of materials contaminated with transuranic is welded, meaning that the fine glassy particles of
isotopes, including items such as protective clothing, the tuff have been fused together by natural heat and
laboratory equipment, used reagents, and solidified pressure. The repository would be sited at a depth of
sludge. The principal radionuclides are plutonium, approximately 350 m in a layer of welded tuff known
americium, and neptunium; small amounts of thor- as the Topapah Spring Member. Above and below
ium, uranium, and other nuclides may also be the repository are layers of nonwelded tuffs that
present. Although the overall radioactivity of TRUW contain few fractures.
is much lower than that of SNF and other high-level Yucca Mountain is located in an arid region,
waste, TRUW contains long-lived radionuclides that where the mean precipitation is less than 20 cm per
remain hazardous for thousands of years. year and an estimated 95% of the water runs off or
The WIPP repository is located in the 240 million- evaporates before it can seep into the ground. The
year-old salt beds of the Permian Salado Formation. water table lies approximately 300 m (1000 feet)
The salt beds are the remains of a shallow saltwater below the level of the repository. Ground water tends
sea that once covered what is now west Texas and to flow to the south toward the Amargosa Desert,
southeastern New Mexico. The Salado Formation is which lies in an isolated hydrological basin having no
200 to 400 m thick, consisting mostly of halite (rock outlet to the ocean.
salt) containing thin layers (0.1–1.0 m thick) of In July 2002, the U.S. Congress voted in favor of a
nonhalite materials such as anhydrite (calcium resolution recommending that Yucca Mountain be
sulfate) and potash. considered for development as a permanent reposi-
The WIPP repository is situated 658 m (2160 feet) tory. At that time, no final design for the repository
below the surface. It comprises a network of had been adopted, but two cases were being
excavations connected to the surface by four vertical considered.
shafts: a salt-handling shaft, a TRUW shaft, an air The base or statutory case would provide an
intake shaft, and an air exhaust shaft. Underground eventual storage capacity of 70,000 metric tons of
roadways called drifts lead from the shafts to the heavy metal (MTHM). The base case repository
waste disposal areas. TRUW is placed in rectangular would store waste containers in 58 tunnels called
rooms that are 4 m high, 10 m wide, and 91 m long. emplacement drifts, each 5.5 m (18 feet) in diameter.
Adjacent rooms are separated by pillars of unexca- The emplacement drifts would be spaced 81 m (266
vated salt that are 31.5 m wide. A group of seven feet) apart, and their total length would be 56,222 m
rooms is called a panel. A total of eight panels are (184,455 feet). An additional 12,988 m (42,612 feet)
planned, but only one had been excavated by the of excavations would be created for access to the
time the first shipment of waste arrived in 1999. repository, with another 6542 m (21,463 feet) of
Other tunnels and rooms have been excavated for excavations being created for the exhaust main.
various scientific experiments. The full inventory case would have a capacity of
97,000 MTHM. It would consist of 90 emplacement
drifts having a total length of 74,214 m (243,484
8.4 Yucca Mountain
feet). The design could be expanded to accommodate
The Yucca Mountain repository is located in the as much as 119,000 MTHM if such expansion ever
Mojave Desert of southern Nevada, approximately becomes necessary.
462 Nuclear Waste