KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo ! 1934 - Fermi irradiates uranium with a neutron source and observes a variety of new radionuclides. This is erroneously interpreted as first evidence of transuranium elements ! 1938 - Hahn and Stra$mann find that the “transuraniumelements” in reality are isotopes of Ba, La etc. ! 1939 - Meitner and Frisch explain this as follows: The nucleus devides into two equally large parts, releasing almost 200 MeV energy, when uranium is irradiated with thermal neutrons ! 1939 - Frisch reports strongly ionising fragments Per Hoff Autumn 2004 Fission, short history Fission, short history Fission, short history ! 1939 - Niels Bohr and John A. Wheeler explain the phenomenon theoretically in simple terms ! 1939 - Bohr explains that thermal fission only occurs with 235U and not with 238U ! 1939 - von Halban and Joliot, as well as Szilard and Fermi, realise that the net gain of neutrons may give a chain reaction, a basis for a reactor ! 1940 - Seaborg, McMillan and Wahl discover Np and Pu, and find that Pu undergoes thernmal neutron fission ! 1942 - Enrico Fermi leads the project building the first nuclear reactor at the Chicago University Stadion. Per Hoff Autumn 2004 ! 1940 - Flerov and Petrzhak discover spontaneous fission ! 1941-45. The Manhattan-district project develops the atomic bomb. Two bombs are used against Japan, one based of isotope enriched 235U, one on reactor produced 239Pu. ! 1956 - First ordinary nuclear power plant, Calder Hall, England, followed by build-up of nuclear power i many contries ! 1960-1962 Extensive fallout from atmospheric bomb tests ! 1963 - Agreement for stopping atmorpheric bomb testing (Moscow treaty) ! 1979 - Harrisburg accident ! 1986 - Tsjernobyl accident Autumn 2004 KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Chain reaction Neutron induced fission Why does fission occur ? Neutron 235 The reason for fission (induced and spontaneous) is that the coulomb forces become stronger than the nuclear forces in large nuclei. A parameter assessing that is the fissionability: Z2/A U 142 91 Ba Kr Neutrons Barium and krypton are examples on fission products which may be formed when the intermediate fissions Autumn 2004 Per Hoff Per Hoff ! Because the number of neutrons produced are larger than the number consumed, one can obtain a chain reaction. ! This was probably first recognised by Leo Szilard. He also tried to patent it. Autumn 2004 Per Hoff Purely energetically, fission is possible wherever energy can be gained by splitting a heavy nucleus into two fragments, but the coulomb barrier prevents that from happening for elements lighter than U. Autumn 2004 Per Hoff KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Energy release in fission Energy release in fission The fission process Consequence; The residual-heat effect 117 The reactor must be cooled also after it is shut down, otherwise the release of heat from the decay of fission products could melt the fuel, eventually making a hole in the reactor tank 234 Energy difference: ~0.9 MeV pr. Nucleon Total energy release pr.fission process is then 4 x ~0.9 = 200 -210 MeV About 180 MeV at fission, the rest is delayed and released as $- and ( Per Hoff Autumn 2004 That happened in the Harrisburg accident 1979. About 50 % of the fuel turned out to be molten, but it did not manage to make a hole in the tank. This accident was the second most serious at a nuclear power plant ever, but did not lead to significant release of radioactivity. But the situation was totally out of control. Per Hoff Autumn 2004 The yield curve is asymmetric with a minimum at 117 Autumn 2004 KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Energy dependence Fission yield Per Hoff Charge dependence 14 MeV Fission neutrons Thermal The lower mass peak moves upwards, when the fissioning mass increases, the upper peak remains. Autumn 2004 Per Hoff When the neutron energy increases, the “valley”is filled for the fission of 235U Autumn 2004 Per Hoff Along a single isobar the yields distribute as whown on this curve, with a maximum at Zp, corresponding to the proton/neutron ratio in the fissioning nucleus Autumn 2004 Per Hoff KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Proton reactions -bismuth Fission products Transuranium elements Fission products are nuclei with a Z/Aratio corresponding roughly to 234U: For A = 139 it gives Zp = 54 (139Xe) For A = 95 it gives Zp = 38 (95Sr) Giving the following sequences 139 Xe(39s) Y 139Cs(2.3m) Y 139Ba(63m) Y139La (stab.) 95 95 95 95 Sr(24s) Y Y(10m) Y Zr(64d) Y Nb(35d) Y 95Mo(stab.) Hence, one gets a waste problem at A= 95, but not atA=139 Autumn 2004 Per Hoff At energies up to 100 MeV there is almost only spallation. Above 100 MeV spallation and high energy fission compete Autumn 2004 Per Hoff Neutron capture in 238U with two consecutive disintegrations give 239Pu as indicated. More neutrons will be captures, and form transuraniums up to 252Cf. Per Hoff Autumn 2004 KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Principle for a nuclear reactor There are many different types of nuclear power plants, from ordinary civilian plants to submarine reactors with very special function. In general, the construction must make it possible to bring the fission process to criticality in a controlled way. This is done by means of control rods made in a material with high ability to capture neutrons with thermal energies, i.e. with high Fthermal, usually Cd or B (as boron carbide) Alsmost all reactors are based on thermal fission. Autumn 2004 Per Hoff ! Consequences: ! One needs a moderator, which slows neutrons down but does not absorb them ! One needs a critical mass of fissile material (235U,233U, 239Pu) ! One needs control rods with high F to control the process ! Produced energy must be removed ! The contruction must give one new neutron available for a new fission after every fission (criticality) ! The process must be controlled, done by means of delayed neutrons ! The neutrons must be slowed down to thermal energies Autumn 2004 Per Hoff Energy release One kg 235U = (1000/235) C 6.02C1023 atoms =2.6C1024 atoms 235U Released energy: 2.6C1024 C 200 MeV = 5.1C1026 MeV = ( 5.1C1026 C1.6C10-13) J = 8.2C1013 J If this amount is developed pr.day, it is released 9.5C108 J pr.second from fission,which implies an effect of 950 MW thermal, a typical average power plant. The electricity production is of course lower, depending upon the transfer efficiency (pure thermodynamics) Autumn 2004 Per Hoff KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Reactor types -boiling water (BWR) Reactor types - Magnox Sketch of swedish pressurised water reactors (Source: SKI) Sketch of swedish boiling water reactors (Source: SKI) Autumn 2004 Reactor types Pressurised water (PWR) Per Hoff Autumn 2004 Per Hoff Per Hoff Autumn 2004 KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Reactor types -Heavy water (Canada) The RBMK-reactor (Tsjernobyl-type) Security barriers T.Henriksen, Biofysikk In this type of reactor, each fuel element stands in a separate channel, surrounded by graphite as moderator material Autumn 2004 Per Hoff Autumn 2004 Per Hoff ! ! ! ! ! ! 1. 2. 3. 4. 5. 6. The fuel itself Fuel encapsulation Reactor vessel Concrete shielding Primary enclosure Bunker Autumn 2004 Per Hoff KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Used fuel Thyroid cancer with children Tsjernobyl accident T.Henriksen. Biofysikk The remains of reactor 4 in Tsjernobyl after the accident The radiologic risk in used fuel declines as shown here. Autumn 2004 Per Hoff Autumn 2004 Per Hoff Kilde: SSI, Sverige It is a dramatic increase in thyroid cancer among persons between 0 and 15 years at the time of the accident, probably due to inferior proptection against exposure to131I Per Hoff Autumn 2004 KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Transport pattern from Tsjernobyl April/May 1986 The weather in this period went from east to west and gave maximum fallout in the district from Gävle to Snåsa Autumn 2004 Per Hoff Radioaktive fallout Waste nuclides ! There are three sources to radioactive waste in a reactor. ! Transuranium nuclides from (n,()processes in the fuel ! Fission products ! Other capture processes (in construction materialser etc.) ! In addition comes waste from the enrichment process, particularly depleted uranium A fallout after an accident will follow different patterns in nature depending on weather, radionuclide chemistry, initial conditions etc. Autumn 2004 Per Hoff Autumn 2004 Per Hoff KJM-5900 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Waste nuclides Most important transuranium isotopes (> 1 Ci pr. Ton used fuel) Halflife > 25 y: 238 Pu 88 y 239 Pu 24 000 y 240 Pu 6560 y 242 ( Pu 375 000 y) 241 Am 432 y 243 Am 7370 y 243 Cm 29 y Halflife 1-25y Pu 14.4 y (soft$, gives 241Am) Cm 18 y 241 244 Per Hoff Autumn 2004 Waste nuclides Most important fission products Very longlived (Halflife > 1000 y) 79 Se 65 000 y 93 Zr 1.5 mill y 99 Tc 213 000 y 107 Pd 6.5 mill y 126 Sn 100 000 y 129 I 16 mill y 135 Cs 2 mill y Methods for final deposit shall prevent also these from release into the environment Autumn 2004 KJM-5900 KJM-5900 Nuclear Chemistry, Dept.of Chem., University of Oslo Nuclear Chemistry, Dept.of Chem., University of Oslo Waste nuclidesSome important shortlived 89 Sr Zr/Nb Ru 131 I 133 I 132 Te 140 Ba 141 Ce 143 Pr 147 Nd 148g,m Pm 149 Pm 151 Pm 153 Sm 95 103 Autumn 2004 Per Hoff Forsmark 1, installation 50 d. 64/35 d 39 d 8d 21 h 3d 13 d (140La daughter) 33 d 14 d 11 d 5/41 d (activation prod.) 2.2 d 1.1 d 2.1 d Per Hoff Autumn 2004 Per Hoff Waste nuclides Most important fission products Average halflife (0.5-100 y) 85 Kr 11 y 90 Sr 29 y (90Y daughter) 106 Ru 1 y (106Rh daughter) 113m Cd 15 y 125 Sb 2.8 y 134 Cs 2.0 y (activation product) 137 Cs 30 y 144 Ce 284d (144Pr daughter) 147 Pm 2.6 y 151 Sm 93 y 154 Eu 8.5 y (activation product) 155 Eu 4.9 y Autumn 2004 Per Hoff
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