Long-lived fission product

Source: Wikipedia, the free encyclopedia.

Long-lived fission products (LLFPs) are radioactive materials with a long

fission reactors
.

Evolution of radioactivity in nuclear waste

activation products from neutron activation
of reactor or environmental materials.

Short-term

The high short-term

radioactivity of spent nuclear fuel is primarily from fission products with short half-life
. The radioactivity in the fission product mixture is mostly due to short-lived isotopes such as 131I and 140Ba, after about four months 141Ce, 95Zr/95Nb and 89Sr constitute the largest contributors, while after about two or three years the largest share is taken by 144Ce/144Pr, 106Ru/106Rh and 147Pm. Note that in the case of a release of radioactivity from a power reactor or used fuel, only some elements are released. As a result, the isotopic signature of the radioactivity is very different from an open air nuclear detonation where all the fission products are dispersed.

Medium-lived fission products

Medium-lived
fission products [further explanation needed]
t½
(year
)
Yield
(%)
keV
)
βγ
155Eu
4.76 0.0803 252 βγ
85Kr 10.76 0.2180 687 βγ
113mCd
14.1 0.0008 316 β
90Sr 28.9 4.505   2826 β
137Cs 30.23 6.337   1176 βγ
121mSn
43.9 0.00005 390 βγ
151Sm
88.8 0.5314 77 β

After several years of cooling, most radioactivity is from the fission products caesium-137 and strontium-90, which are each produced in about 6% of fissions, and have half-lives of about 30 years. Other fission products with similar half-lives have much lower fission product yields, lower decay energy, and several (151Sm, 155Eu, 113mCd) are also quickly destroyed by neutron capture while still in the reactor, so are not responsible for more than a tiny fraction of the radiation production at any time. Therefore, in the period from several years to several hundred years after use, radioactivity of spent fuel can be modeled simply as exponential decay of the 137Cs and 90Sr. These are sometimes known as medium-lived fission products.[1][2]

Krypton-85, the 3rd most active MLFP, is a noble gas which is allowed to escape during current nuclear reprocessing; however, its inertness means that it does not concentrate in the environment, but diffuses to a uniform low concentration in the atmosphere. Spent fuel in the U.S. and some other countries is not likely to be reprocessed until decades after use, and by that time most of the 85Kr will have decayed.

Actinides

Actinides[3] by decay chain Half-life
range (a)
Fission products of 235U by yield[4]
4n
4n + 1
4n + 2
4n + 3
4.5–7% 0.04–1.25% <0.001%
228
Ra
4–6 a
155
Euþ
244
Cmƒ
241Puƒ
250
Cf
227
Ac
10–29 a
90Sr 85Kr
113m
Cdþ
232Uƒ 238Puƒ
243
Cmƒ
29–97 a
137
Cs
151
Smþ
121m
Sn
248Bk[5]
249
Cfƒ
242m
Amƒ
141–351 a

No fission products have a half-life
in the range of 100 a–210 ka ...

241Amƒ
251Cfƒ[6]
430–900 a
226Ra
247
Bk
1.3–1.6 ka
240Pu
229
Th
246
Cmƒ
243
Amƒ
4.7–7.4 ka
245
Cmƒ
250
Cm
8.3–8.5 ka
239Puƒ 24.1 ka
230
Th
231
Pa
32–76 ka
236
Npƒ
233Uƒ 234U 150–250 ka 99Tc
126
Sn
248
Cm
242Pu 327–375 ka 79Se
1.53 Ma
93
Zr
237
Npƒ
2.1–6.5 Ma
135
Cs
107
Pd
236U
247
Cmƒ
15–24 Ma 129I
244Pu 80 Ma

... nor beyond 15.7 Ma[7]

232Th 238U 235Uƒ№ 0.7–14.1 Ga
(thermal neutron capture cross section greater than 3k barns)

After 137Cs and 90Sr have decayed to low levels, the bulk of radioactivity from spent fuel come not from fission products but

fusion reactors. Americium-241 has some industrial applications and is used in smoke detectors
and is thus often separated from waste as it fetches a price that makes such separation economic.

Long-lived fission products

On scales greater than 105 years, fission products, chiefly

, if those have not been destroyed.

The most abundant long-lived fission products have total decay energy around 100–300 keV, only part of which appears in the beta particle; the rest is lost to a neutrino that has no effect. In contrast, actinides undergo multiple alpha decays, each with decay energy around 4–5 MeV.

Only seven fission products have long half-lives, and these are much longer than 30 years, in the range of 200,000 to 16 million years. These are known as long-lived fission products (LLFP). Three have relatively high yields of about 6%, while the rest appear at much lower yields. (This list of seven excludes isotopes with very slow decay and half-lives longer than the age of the universe, which are effectively stable and already found in nature, as well as a few nuclides like technetium-98 and samarium-146 that are "shadowed" from beta decay and can only occur as direct fission products, not as beta decay products of more neutron-rich initial fission products. The shadowed fission products have yields on the order of one millionth as much as iodine-129.)

The 7 long-lived fission products

Nuclide
t12
Yield Q[a 1]
βγ
(
Ma
)
(%)[a 2] (
keV
)
99Tc 0.211 6.1385 294 β
126Sn
0.230 0.1084 4050[a 3] βγ
79Se 0.327 0.0447 151 β
135Cs
1.33 6.9110[a 4] 269 β
93Zr
1.53 5.4575 91 βγ
107Pd
6.5   1.2499 33 β
129I 15.7   0.8410 194 βγ
  1. ^ Decay energy is split among β, neutrino, and γ if any.
  2. ^ Per 65 thermal neutron fissions of 235U and 35 of 239Pu.
  3. ^ Has decay energy 380 keV, but its decay product 126Sb has decay energy 3.67 MeV.
  4. ^ Lower in thermal reactors because 135Xe, its predecessor, readily absorbs neutrons.

The first three have similar half-lives, between 200 thousand and 300 thousand years; the last four have longer half-lives, in the low millions of years.

  1. , TcO4) that are relatively mobile in the environment.
  2. thermal neutrons, so the energy per unit time from 126Sn is only about 5% as much as from 99Tc for U-235 fission, or 20% as much for 65% U-235+35% Pu-239. Fast fission may produce higher yields. Tin
    is an inert metal with little mobility in the environment, helping to limit health risks from its radiation.
  3. Selenium-79 is produced at low yields and emits only weak radiation. Its decay energy per unit time should be only about 0.2% that of Tc-99.
  4. Zirconium-93 is produced at a relatively high yield of about 6%, but its decay is 7.5 times slower than Tc-99, and its decay energy is only 30% as great; therefore its energy production is initially only 4% as great as Tc-99, though this fraction will increase as the Tc-99 decays. 93Zr does produce gamma radiation, but of a very low energy, and zirconium
    is relatively inert in the environment.
  5. 137Cs
    which does not absorb neutrons but is highly radioactive, making handling more hazardous and complicated; for all these reasons, transmutation disposal of 135Cs would be more difficult.
  6. Palladium-107 has a very long half-life, a low yield (though the yield for plutonium fission is higher than the yield from uranium-235 fission), and very weak radiation. Its initial contribution to LLFP radiation should be only about one part in 10000 for 235U fission, or 2000 for 65% 235U+35% 239Pu. Palladium is a noble metal
    and extremely inert.
  7. billion
    times as long as its more hazardous sister isotope 131I; therefore, with a shorter half-life and a higher decay energy, 131I is approximately a billion times more radioactive than the longer-lived 129I. (What relevance 131I has in this coverage of LLFPs is debatable.)

LLFP radioactivity compared

In total, the other six LLFPs, in thermal reactor spent fuel, initially release only a bit more than 10% as much energy per unit time as Tc-99 for U-235 fission, or 25% as much for 65% U-235+35% Pu-239. About 1000 years after fuel use, radioactivity from the medium-lived fission products Cs-137 and Sr-90 drops below the level of radioactivity from Tc-99 or LLFPs in general. (Actinides, if not removed, will be emitting more radioactivity than either at this point.) By about 1 million years, Tc-99 radioactivity will have declined below that of Zr-93, though immobility of the latter means it is probably still a lesser hazard. By about 3 million years, Zr-93 decay energy will have declined below that of I-129.

cross sections, although transmutation is still slow compared to fission of actinides in a reactor. Transmutation has also been considered for Cs-135, but is almost certainly not worthwhile for the other LLFPs. Given that stable Caesium-133 is also produced in nuclear fission and both it and its neutron activation product 134
Cs
are neutron poisons, transmutation of 135
Cs
might necessitate isotope separation. 99
Tc
is particularly attractive for transmutation not only due to the undesirable properties of the product to be destroyed and the relatively high neutron absorption cross section but also because 100
Tc
rapidly beta decays to stable 100
Ru
. Ruthenium
has no radioactive isotopes with half lives much longer than a year and the price of ruthenium is relatively high, making the destruction of 99
Tc
into a potentially lucrative source of producing a precious metal from an undesirable feedstock.

References

  1. .
  2. ^ Zerriffi, Hisham; Makhijani, Annie (May 2000). "The Nuclear Alchemy Gamble: An Assessment of Transmutation as a Nuclear Waste Management Strategy". Institute for Energy and Environmental Research.
  3. ^ Plus radium (element 88). While actually a sub-actinide, it immediately precedes actinium (89) and follows a three-element gap of instability after polonium (84) where no nuclides have half-lives of at least four years (the longest-lived nuclide in the gap is radon-222 with a half life of less than four days). Radium's longest lived isotope, at 1,600 years, thus merits the element's inclusion here.
  4. thermal neutron fission of uranium-235, e.g. in a typical nuclear reactor
    .
  5. .
    "The isotopic analyses disclosed a species of mass 248 in constant abundance in three samples analysed over a period of about 10 months. This was ascribed to an isomer of Bk248 with a half-life greater than 9 [years]. No growth of Cf248 was detected, and a lower limit for the β half-life can be set at about 104 [years]. No alpha activity attributable to the new isomer has been detected; the alpha half-life is probably greater than 300 [years]."
  6. sea of instability
    ".
  7. ^ Excluding those "classically stable" nuclides with half-lives significantly in excess of 232Th; e.g., while 113mCd has a half-life of only fourteen years, that of 113Cd is eight quadrillion years.