Long-lived fission product
Long-lived fission products (LLFPs) are radioactive materials with a long
Evolution of radioactivity in nuclear waste
Short-term
The high short-term
Medium-lived fission products
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) |
|||||||
---|---|---|---|---|---|---|---|---|
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 | ||||
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 | |||||
|
After 137Cs and 90Sr have decayed to low levels, the bulk of radioactivity from spent fuel come not from fission products but
Long-lived fission products
On scales greater than 105 years, fission products, chiefly
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 | t1⁄2
|
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 |
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.
- anions (pertechnetate, TcO4−) that are relatively mobile in the environment.
- 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. Tinis an inert metal with little mobility in the environment, helping to limit health risks from its radiation.
- 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.
- 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 zirconiumis relatively inert in the environment.
- 137Cswhich 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.
- 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 metaland extremely inert.
- billiontimes 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.
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
Tc into a potentially lucrative source of producing a precious metal from an undesirable feedstock.
References
- ISBN 978-0-309-05226-9.
- ^ 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.
- ^ 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.
- thermal neutron fission of uranium-235, e.g. in a typical nuclear reactor.
- .
"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]." - sea of instability".
- ^ 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.