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THE NUCLEAR WASTE PROBLEM

A typical 1000 MWe PWR reactor operating at 75% capacity generates about 21 tons of spent fuel at a burn-up of 43 GWd/t. The 21 tons of spent fuel (contained inside 42 PWR fuel elements with a total volume of about 11 m3) will have produced an electric energy of about 6.6 TWh (6.6 billion kWh). This same energy output corresponds to the burning of 2 million tons of coal in a conventional power plant giving rise to 120,000 tons of ashes, 5.4 million tons of CO2 and 50,000 tons of SO2.5 Spent fuel consists of uranium which accounts for about 96% of the spent fuel removed from commercial nuclear reactors. In the case of light water reactors (the type most commonly used) the spent fuel contains 0.90% U235 whereas natural uranium contains only 0.70% of this isotope. Plutonium constitutes about 1% of the weight of spent fuel; it is fissile which means that it can be used as fuel in nuclear reactors. The minor actinides constitute about 0.1% of the weight of spent fuel. They consist of about 50% Np, 47% Am and 3% Cm which are very radiotoxic. The fission products (iodine, technetium, neodymium, zirconium, molybdenum, cerium, cesium, ruthenium, palladium, etc.) constitute about 2.9% of the weight of spent fuel. The two fission products of principal concern because of their substantial thermal impact on the repository as opposed to posing a health risk are Sr90 and Cs137. These two radionuclides are dominant contributors to the heat released by spent fuel at least for the first several decades. Cs137 is also a major source of penetrating radiation emitted by spent fuel. The two fission products of principal concern because of their potential contribution to health risk are Tc99 and I129. They are of principal concern because they are long-lived, produced in significant amounts in the fission process, generally soluble under geologic conditions, and migrate relatively quickly under common ground water conditions. The long-term toxicity of spent fuel is dominated by the actinides such as Np237, U234, 236, and Pu239, 240,242. The transmutation of long-lived nuclides in high level waste to stable or short-lived nuclides by stimulating nuclear reactions is a desirable alternative approach for the reduction of high level waste. There are about 300 different radioactive species generated by the operation of a nuclear reactor, primarily as a result of neutron capture and neutron-induced fission. The adverse impact of the various radionuclides varies because of the differences in the chemical behavior in the body of, and the radiation emitted by, the radionuclides. The risk focus of the
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rather 2 . transport of radionuclides to the accessible environment. This strategy is called transmutation • THE SOLUTION: SUB-CRITICAL ACCELERATOR DRIVEN REACTOR Since the early 1990s.000 years.e. Sr90. The management of spent fuel should ensure that the biosphere is protected under economically acceptable conditions without entailing unfavorable short-term consequences and the public must be convinced of the effectiveness of the methods. Two means are possible: 1. We can make use of nuclear reactions that will transmute the very long-lived wastes into less radioactive or shorter-lived products. The reaction is not driven by the well known self sustained. Although hundreds of isotopes are present in spent fuel or wastes derived from them. I129 and Tc99 are the primary focus of concern for light-water reactor spent fuel. chain-reaction. some protection is required for at least 100. Since the spent fuel contains very long-lived radionuclides. i. and critically evaluating the state of accelerator. Although the concept of accelerator-driven systems has been proposed before under different circumstances. high-power accelerators for an alternative solution to the disposition of nuclear waste. Los Alamos National Laboratory (LANL) has led the development of accelerator-driven transmutation of waste (ATW) to provide an alternative technological option to the disposition of nuclear waste. or health risk. only a few of them are important for disposal. The most common release and exposure mechanisms from a repository involve ground water contacting the waste form followed by slow dissolution. 2.. These four isotopes Cs137. nuclear waste due to their excess heat. The photon reactor is a method and means for producing nuclear energy from heavy elements but not fissile elements. groundwater solubility. it has only become technically feasible in recent years due to the advent of high-current. nuclear and processing technologies. We can wait for the natural decay of the radioactive elements by isolating them physically from the biosphere by installing successive barriers at a suitable depth in the ground. distribution in the biosphere.radionuclides is related to waste disposal in a geologic repository. and eventual uptake from food and water. of U235. This strategy is called deep geological disposal.

Patents are currently pending. four spaced accelerators would require about 4. Chemical separations of the spent fuel isotopes is not necessary. A linear accelerator. the threshold of photofission is about 6 MeV and results in fission of the U238 nucleus releasing about 200 MeV. accelerates electrons which are directed onto a high Z target such as tungsten to generate gamma rays of an energy about 10 MeV. more than one accelerator may be used to drive the reactor to higher power levels. Figure 1:The accelerator driven reactor schematic 3 . The fuel for this type of accelerator driven reactor may be the spent fuel from fission reactors. and speed-up the burn-up process.n) reaction resulting in short lived or stable products.by an accelerator. Of course. with U238. The photo-fission results in typical spent fuel waste products such as Cs137 and Sr90 which undergo photodisintegration by the (γ. A reactor built according to this principle requiring an accelerator driven by 1 MW will develop about 20 MW of power.f) reaction. The reaction is not self-sustaining and stops when the beam is turned off. if simply operated at 10 MeV. wherein a photon or gamma is introduced greater than the photo-fission threshold energy resulting in fission of the target nucleus.8 MW of power to run resulting in about 100 MW from the reactor. thus releasing about 200 MeV. Ideally. which are directed onto the fuel material such as U238 which results in the (γ. This accelerator driven reactor may be used to "burnup" spent fuel from fission reactors. For instance. preferably of the monochromatic type. The mechanism by which nuclear energy is released from non-fissile material is known as photo-fission.

• · The R&D during and after the Integral Fast Reactor (IFR) program at Argonne National Laboratory. · Produce electricity. **Advances in the following three fields contribute to establishing the feasibility of such an ATW system: · The Accelerator Production of Tritium (APT) program has begun the engineering design and testing of a high-power accelerator one more powerful than is needed for ATW.7 the plutonium preprocessing experience at Los Alamos. The ATW resembles a nuclear reactor in that it releases energy during actinide fission that can be converted into electricity.To make an impact on the disposition of nuclear waste. they will be separated from the remainder of the waste and placed in optimised storage systems.9% of the technetium (Tc) and iodine (I). · Separate uranium. Their elimination also greatly reduces long-term heat loading in the repository. an ATW system should accomplish the following: • • • • • · Destroy over 99.11 has allowed the conceptualization of integral • 4 . Uranium is separated from the rest of the spent fuel. Sr-90 and Cs-137 dominate the short-term heat loading in the repository. Fissioning the TRUs eliminates concerns related to their release to the ground water and the environment as well as their possible diversion and use for weapons. and achieve the necessary degree of TRU removal from the waste stream destined for final disposition.9% of thelong-lived transuranic elements (TRUs). A small fraction (10–15%) of this electricity will be used to power the accelerator and the rest can be distributed. and either stored or possibly re-enriched for use in conventional reactors. Two of the long-term radiotoxic hazards can be eliminated by transmuting these elements. and although these isotopes are not suited for transmutation. · Separate Sr and Cs (short half-life isotopes). • · The recently released Russian lead–bismuth (LBE) nuclear coolant technology10.8 and other efforts worldwide to develop preprocesses have given us the capability to treat spent nuclear fuels and ATW waste in a much simplified and proliferationresistant manner. · Destroy over 99.

The end products of ATW are a more benign fission product waste stream. This approach contrasts with the present-day reprocessing practices in Europe and Japan. ATW would inhibit plutonium accumulation.nf) peaks. As such. as is the case for essentially all medium and heavy nuclei as provided by the examples in figure 3 5 . proliferation and diversion. These neutron reactions result in additional energy output thereby increasing the input/output ratio from 1/20 a value determined by the design. uranium similar in composition to natural uranium. and safer reactor technologies REACTIONS IN THE ACCELERATOR DRIVEN REACTOR It is important to note that although the reactor is sub-critical and driven by gamma rays. could offset to some extent the cost of developing and implementing the technology. and the potential cost benefits realized by enhancing the capacity of a repository and elimination of the need for an additional repository. this appears to hold true for all the actinides.spallation (decay caused by high energy particle bombardment) target and blanket systems with excellent transmutation efficiency. other transuranics and selected long-lived fission products would be destroyed by fission or transmutation in the facility. Far from being limited to waste destruction. The maximum cross sections are all about 0. Notice that the total photonuclear cross sections all have about the same peak cross section value. or reducing the long-term performance uncertainties. in which high purity plutonium is produced and used in the fabrication of fresh mixed-oxide (MOX) fuel that is shipped offsite for use in LWRs. Instead of reprocessing. ATW has gained worldwide interest and could become an important component of strategies to deal with international nuclear materials management and promote new. The photo-absorption cross section falls sharply above the (γ. the ATW approach can be characterized as once-through destruction. ATW technology also brings to the table new concepts that could be relevant for nextgeneration power producing systems. Figure 2 shows the photonuclear cross sectional data obtained by Veyssiere for U238. spent fuel would be shipped to an ATW site where the plutonium. The electricity produced.5 b and all are about 6 MeV wide. the neutrons produced still induce both fast and slow neutron fission just as in any conventional reactor. In the ATW concept.2N) and (γ. proliferation-resistant. and electricity.

n). U238 and Np237 6 .Figure 2.f).tot) for U238. Partial and total photonuclear cross sections (γ . and (γ . Figure 3. (γ .2n). (γ . Total photonuclear cross sections for Th232.

n) ENRICHMENT: 92U236 + γ 92U235 + 0n1 92U238 + γ 92U236 + 2 0n1 + γ 92U235 + 0n1 95Am241 + γ 95Am240 + 0n1 + -1e0 94Pu240 93Np237 + γ 93Np235 + 2 0n1 + -1e0 92U235 92U238 + γ 92U237 + 0n1 + γ 92U236 + 0n1 + γ 92U235 + 0n1 94Pu238 + γ 94Pu236 + 2 0n1 + γ 94Pu235 + 0n1 + -1e0 93Np235 + -1e0 92U235 92U238 + γ 92U237 + 0n1 93Np237 + β .n) NEUTRALIZATION: 1H3 + γ 1H2 + 0n1 (stable) 6C14 + γ 6C13 + 0n1 (stable) 39Y90 + γ 39Y89 + 0n1 (stable) 28Ni63 + γ 28Ni62 + 0n1 (stable) 36Kr85 + γ 36Kr84 + 0n1 (stable) 27Co60 + γ 27Co59 + 0n1 (stable) 81Tl204 + γ 81Tl203 + 0n1 (stable) 38Sr90 + γ 38Sr88 + 2 0n1 (stable) 83Bi210 + γ 83Bi209 + 0n1 (stable) 56Ba133 + γ 56Ba132 + 0n1 (stable) 82Pb210 + γ 82Pb208 + 2 0n1 (stable) 38Sr90 + γ 38Sr89 + 0n1 39Y89 + β . U231.(stable) 53I129 + γ 53I128 + 0n1 54Xe128 + β . Pu241. of course.(stable) 54Xe140 55Cs140 + β -56Ba140 + β -57La140 + β -58Ce140 + β (stable) (γ .+ γ 93Np235 + 2 0n1 + -1e0 92U235 94Pu239 + γ 94Pu237 + 2 0n1 + γ 94Pu235 + 2 0n1 + -1e0 93Np235 + -1e0 92U235 94Pu239 + γ 92U235 + α NEUTRON ENRICHMENT: 92U234 + 0n1 92U235 + γ 92U238 + 0n1 92U239 + γ 93Np239 + β -94Pu239 + β 90Th232 + 0n1 90Th233 + γ 91Pa233 + β -92U233 + β (γ . In addition. U235. Pa232. Th232. U231. Th227. FISSION REACTIONS: (just one of many) 92U235 + 0n1 38Sr94 + 54Xe140 + 2 0n1 38Sr94 39Y94 + β -40Zr94 + β . accelerator driven reactor are too numerous to list but the most important reactions are shown in Table 1 PHOTOFISSION REACTIONS: (γ . f) reaction.n) reaction is about three times the (γ. Pu239. Pa232. Th227. Pu239. U233. Np238.The thermal fissionable nuclides include Np238. Th232. f): U238. All those nuclides fissionable by thermal neutrons are. there are several nuclides such as U238. Pa231. U233. Pa231. also fissionable by fast neutrons. U235.(stable) 7 . Pu241. Looking at figures 3 through 5 we see that at 10 MeV the (γ. and Np237 which are fissionable by neutrons having energies of about 1 MeV. Np237.

The accelerator was designed for 40 MW in order to be able to drive up to a total 2000 MWt fission power. This structure has revolutionized the ability to transport high quality beams from an RFQ to following structures.High-Power Linear Accelerator The 1000MeV reference linac design for ATW is based on consideration of a number of important issues. The ATW linac length is 355 m. insensitivity to errors in alignment and settings. The design uses demonstrated components to transmit the beam through the different energy regimes. high efficiency of electrical power to beam power conversion. A suitable injector has been working for months at LANL with currents (110 mA) in excess of a factor of two for what ATW needs and with beam parameters better than the ATW requirements to ensure low beam loss. and previous tests with these lower beta structures showed their benefits.2 MeV beam from the CCDTL is then fed into a set of superconducting cavities that take the beam up to 1000 MeV. reliable operations. The 21. 8 .3 MW for a 40 MW beam. Following the RFQ is a coupled cavity drift tube linac (CCDTL) that will be demonstrated in the APT Low Energy Demonstration Accelerator (LEDA) program.7 MeV in a radio frequency quadrupole (RFQ) based on a well-defined beam emerging from a reliable injector. and cost optimization. These include low beam losses. Initially the beam is accelerated to 6. which could be distributed within one 500–1000 MWt system. The first type of cavity that accelerates the beam to 100 MeV is based on a “spoke” resonator design that will require some testing before it is fully qualified for this program. In addition. the CRITS (Chalk River Injector Test Stand) RFQ has been accelerating a proton beam with good transmission and beam parameters exceeding the ATW requirements. All indications are that there should be no problems with this geometry because there should be no problems with the required field levels in the cavities. The last stage of acceleration will be with elliptical shaped cavities: these have been demonstrated to be able to meet the required performance regimes necessary for ATW. with a radio frequency power need of 42.

946 Transmission (load) 0.8 Gain 50 dB Efficiency 65% Modulation Modulating Anode Table 2-Accelerator Specifications 9 .850 Multiplication (no load) 3.0 Multiplication (load) 2.0 MV/m Number of Accelerator Guides 7 Resonant Ring Transmission (no load) 0.2 MW Beam Voltage 90 KV Micro-Perveance 0.4 MV/m to 2.0 Klystron Number of klystrons 2 Power 1.General Operation Mode Continuous Wave Energy 10 MeV Beam Current 100 mAmp Total Length 18 meters Normal Emittance 50% mm mrad Energy Spread 1% Accelerator Section Type Traveling Wave Constant-Gradient Mode 2p/3 Frequency 1249.135 MHz Gain (max) 1.

(Eq. λ i = decay constant of the ith nucleus.(6) is written as follows: dN/dt = A · N. CONCLUSION The (γ. Using the matrix representation. Kase ran the feasibility experiment that provided proof of feasibility on the laboratory scale.n) incineration of spent nuclear fuel provides an efficient and reasonable method for disposal of radioactive waste while providing a relatively cheap and safe source of power at the same time.BEAM FLUX REQUIREMENTS Calculations show that efficient (γ.2.…. f) and (γ.n) reacting during the irradiation can be determined by the following differential equation: dNi/dt = -( λ i + ði Φ) Ni + Σ (λ lji + ðji Φ) Nj .n) incineration of Cs137 and Sr90 requires a gamma flux of but only 1018 g/cm2sec to accelerate the time of decay by 180 times The number of nuclei (γ. 1) i = 1. Safety is high. ði = total photonuclear cross section of the ith nucleus λji = decay constant from the jth nucleus transmuting to the ith one. Na where Ni = number of the ith nucleus. Such a reactor may be fueled by current nuclear waste stockpiles. where -(λi + ði f) (i = j). A small proof of principle accelerator driven reactor could be build using known engineering with reasonable assurance and confidence that it will work as designed. now all that remains is to apply the technology and build an experimental accelerator driven reactor. Σji = { λji + ðji Φ (i ¹ j). natural U238 or natural Th232. Matsumoto ran the calculations to show it is theoretically feasible. spent nuclear fuel. eq. ð = g-ray flux. Na = number of nuclei considered in the model. 2) 10 . No new technology needs to be developed since we currently have all the required technology available to us. (Eq. fuel is cheap and abundant.

The Uranium Institute 24th Annual Symposium: London 8-10 September 1999 2) P. Disposition of Nuclear Wastes Using Subcritical Accelerator-Driven Systems . et. Venneri. The Photon Reactor: Producing Power By Burning Nuclear Waste.al.M Brown .REFERENCES 1) F. LLC 11 . Nuclear Solutions.