Fuel Depletion – Isotopic Changes

Fuel Depletion - Isotopic Changes

Isotopic changes of 4% uranium-235 fuel as a function of fuel burnup.

As a reactor is operated at significant power, atoms of fuel are constantly consumed, resulting in the slow depletion of the fuel. It must be noted there are also research reactors, which have very low power and the fuel in these reactors does not change its isotopic composition.

Research reactors with significant thermal power and all power reactors are subjected to significant isotopic changes. The study of these isotopic changes is known as the long-term kinetics, which describes phenomena that occur over months or even years. The study of phenomena that occur over the course of several hours to a few days, for example, effects of neutron poisons on the reactivity (i.e. Xenon poisoning or spatial oscillations), is known as the medium-term kinetics.
This chapter describes the long-term kinetics of thermal reactors based on the uranium fuel cycle, in which a fuel with a large concentration of uranium-238 is used (e.g. PWRs or BWRs).  Most common reactor fuels are composed of either natural or partially enriched uranium. Typically, PWRs uses an enriched uranium fuel (~4% of U-235) as a fresh fuel. Exposure to neutron flux gradually depletes the uranium-235, decreasing core reactivity (compensated by control rods, chemical shim or burnable absorbers). The initial fuel load of a new reactor core (so called first core) is entirely fresh fuel, that is, fuel with no plutonium or fission products present. The contribution of uranium-238 directly to fission is quite small in most thermal reactors. On the other hand uranium-238 plays very important role and this chapter is primarily about this isotope.

See also: Uranium

See also: Plutonium

Fissile / Fertile Material Cross-sections

Source: JANIS (Java-based nuclear information software)
http://www.oecd-nea.org/janis/

is a fissile isotope and its fission cross-section for thermal neutrons is about 585 barns (for 0.0253 eV neutron). For fast neutrons its fission cross-section is on the order of barns. Most of absorption reactions result in fission reaction, but a minority results in radiative capture forming 236U. The cross-section for radiative capture for thermal neutrons is about 99 barns (for 0.0253 eV neutron). Therefore about 15% of all absorption reactions result in radiative capture of neutron. About 85% of all absorption reactions result in fission.

Uranium absorption reaction

Fissile / Fertile Material Cross-sections

Fissile / Fertile Material Cross-sections. Uranium 238.
Source: JANIS (Java-based nuclear information software)
http://www.oecd-nea.org/janis/

238U is a fissionable isotope, but is not fissile isotope. 238U is not capable of undergoing fission reaction after absorbing thermal neutron, on the other hand 238U can be fissioned by fast neutron with energy higher than >1MeV. During the fuel burning, the content of the U-235 continuously decreases and the content of the plutonium increases (up to ~1% of Pu ). 238U belongs also to the group of fertile isotopes. Radiative capture of a neutron leads to the formation of fissile 239Pu and other transuranic elements. This is the way how 238U contributes to the operation of nuclear reactors and production of electricity through this plutonium. For example, at a burnup of 40GWd/tU, about 40% of the total energy released comes from bred plutonium. This corresponds to a breeding ratio for this fuel burnup of about 0.4 to 0.5. That means, about half of the fissile fuel in these reactors is bred there. This effect extends the cycle length for such fuels to sometimes nearly twice what it would be otherwise. MOX fuel has a smaller breeding effect than 235U fuel and is thus more challenging and slightly less economic to use due to a quicker drop off in reactivity through cycle life.

Equation - Plutonium 239 breeding from Uranium 238

Fissile / Fertile Material Cross-sections

Source: JANIS (Java-based nuclear information software)
http://www.oecd-nea.org/janis/

Plutonium 239 is a fissile isotope and its fission cross-section for thermal neutrons is about 750 barns (for 0.025 eV neutron). For fast neutrons its fission cross-section is on the order of barns. Most of absorption reactions result in fission reaction, but a part of reactions result in radiative capture forming 240Pu. The cross-section for radiative capture for thermal neutrons is about 270 barns (for 0.025 eV neutron). Therefore about 27% of all absorption reactions result in radiative capture of incident neutron. About 73% of all absorption reactions result in fission.

Plutonium fission vs. radiative capture

Fissile / Fertile Material Cross-sections

Source: JANIS (Java-based nuclear information software)
http://www.oecd-nea.org/janis/

241Pu is a fissile isotope, which means 241Pu is capable of undergoing fission reaction after absorbing thermal neutron. Moreover 241Pu meets also alternative requirement that the amount of neutrons produced by fission of 241Pu (~2.94 per one fission by thermal neutron) is sufficient to sustain a nuclear fission chain reaction. Its fission cross-section for thermal neutrons is about 1012 barns (for 0.025 eV neutron). For fast neutrons its fission cross-section is on the order of barns. Most of absorption reactions result in fission reaction, but a part of reactions result in radiative capture forming 242Pu. The cross-section for radiative capture for thermal neutrons is about 363 barns (for 0.025 eV neutron). Therefore about 74% of all absorption reactions result in radiative capture of neutron. About 26% of all absorption reactions result in fission. 241Pu decays via beta decay into 241Am with half-life of only 14.3 years. 241Am has relatively high cross-section for radiative capture for thermal neutrons (~680 barns – 0.025eV). This two phenomena (decrease in fissile isotope and increase in neutron absorber) cause slight decrease in reactivity of irradiated fuel when stored in a spent fuel pool.

Evolution Equations

The exact evolution of isotopic changes is usually modelled mathematically a set of differential equations known as evolution equations. These equations describe the rate of burnup of U-235, the rate of buildup of Pu-239, production of Pu-240 and Pu-241, the buildup of neutron absorbing fission products, and the overall rate of reactivity change in the reactor due to the changing composition of the fuel. The evolution equation can be constructed for each isotope. For example:

Evolution Equations

Special reference: W. M. Stacey, Nuclear Reactor Physics, John Wiley & Sons, 2001, ISBN: 0- 471-39127-1.

Special reference: Paul Reuss, Neutron Physics, EDP Sciences, 2008, ISBN: 2759800415.

Isotopic Changes – Summary

Fuel Depletion - Isotopic Changes

Isotopic changes of 4% uranium-235 fuel as a function of fuel burnup.

In summary, it can be seen for fuel burnup of 40 GWd/tU:

  • Approximately 3 – 4% of the heavy nuclei are fissioned.
  • About two thirds of these fissions come directly from uranium 235, and the other third from plutonium, which is produced from uranium 238. The contribution significantly increases as the fuel burnup increases.
  • The removed fuel (spent nuclear fuel) still contains about 96% of reusable material. It must be removed due to decreasing kinf of an assembly or in or in other words, it must be removed due to accumulation of fission products with significant absorption cross-section.
  • Discharged fuel contains abour 0.8% of plutonium and about 1% of uranium 235. It must be noted, there is a significant content (about 0.5%) of uranium 236, which is is neither a fissile isotope, nor a fertile isotope.

Effect of Fuel Depletion on the Power Distribution

During operation of a reactor the amount of fissile material contained in the fuel assembly constantly decreases, therefore the assembly kinf constantly decreases. During fuel depletion the decrease of the assembly kinf will be greatest where the power is greatest. The differences in kinf between fresh fuel assemblies and high-burnup assemblies decreases. Therefore during cycle depletion, this process will cause the power to shift away from regions with highest kinf. This process also depends on the use of burnable absorbers, which disrupt the first assumption about the constantly decreasing assembly kinf.

Effect of Fuel Depletion on Delayed Neutrons

In LWRs the delayed neutron fraction decreases with fuel burnup. This is due to isotopic changes in the fuel. It is simple, fresh uranium fuel contains only 235U as the fissile material, meanwhile during fuel burnup the importance of fission of 239Pu increases (in some cases up to 50%). Since 239Pu produces significantly less delayed neutrons (0.0021 vs. 0.0064), the resultant core delayed neutron fraction of a multiplying system decreases (it is the weighted average of the constituent delayed neutron fractions). It follows then that the amount of reactivity insertion needed to produce a given reactor period decreases with burnup of the fuel. This is also the reason why the neutron spectrum in the core become harder with fuel burnup.

βcore= ∑ Pii

where Pi is fraction of power generated by isotope i.

Reactivity Effects of Fuel Burnup

infinite multiplication factor - nuclear fuel↑burnup ↓keff = ↓η  .ε.p.  ↓f  .  ↑↓Pf.  ↑↓Pt

It is hard to describe the effects of fuel burnup on the six factor formula. It must be noted, the criticality must be maintained for long period and therefore all the negative effects must be compensated by the increase in the thermal utilization factor (boron dilution or compensating rods withdrawal).

See more: Operational factors that affect the multiplication

Nuclear and Reactor Physics:

  1. J. R. Lamarsh, Introduction to Nuclear Reactor Theory, 2nd ed., Addison-Wesley, Reading, MA (1983).
  2. J. R. Lamarsh, A. J. Baratta, Introduction to Nuclear Engineering, 3d ed., Prentice-Hall, 2001, ISBN: 0-201-82498-1.
  3. W. M. Stacey, Nuclear Reactor Physics, John Wiley & Sons, 2001, ISBN: 0- 471-39127-1.
  4. Glasstone, Sesonske. Nuclear Reactor Engineering: Reactor Systems Engineering, Springer; 4th edition, 1994, ISBN: 978-0412985317
  5. W.S.C. Williams. Nuclear and Particle Physics. Clarendon Press; 1 edition, 1991, ISBN: 978-0198520467
  6. G.R.Keepin. Physics of Nuclear Kinetics. Addison-Wesley Pub. Co; 1st edition, 1965
  7. Robert Reed Burn, Introduction to Nuclear Reactor Operation, 1988.
  8. U.S. Department of Energy, Nuclear Physics and Reactor Theory. DOE Fundamentals Handbook, Volume 1 and 2. January 1993.

Advanced Reactor Physics:

  1. K. O. Ott, W. A. Bezella, Introductory Nuclear Reactor Statics, American Nuclear Society, Revised edition (1989), 1989, ISBN: 0-894-48033-2.
  2. K. O. Ott, R. J. Neuhold, Introductory Nuclear Reactor Dynamics, American Nuclear Society, 1985, ISBN: 0-894-48029-4.
  3. D. L. Hetrick, Dynamics of Nuclear Reactors, American Nuclear Society, 1993, ISBN: 0-894-48453-2. 
  4. E. E. Lewis, W. F. Miller, Computational Methods of Neutron Transport, American Nuclear Society, 1993, ISBN: 0-894-48452-4.

See above: