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its own bayonet-style partial internal flange which allows the crucible ring to be rotated and locked onto the crucible bottom. This allows the crucible assembly to be transferred into and out of the furnace as a single piece, but separated for ingot dumping. The crucible ring and crucible bottom are constructed of graphite lined with aluminum oxide refractory, which is non-wetting to molten metal and resistant to damage from reactive molten chlorides. Figure 8-12. Metal Waste Form Furnace The cladding hulls with the appropriate amount of zirconium added are loaded into a thin-walled stainless steel container and placed inside the crucible assembly. The crucible is then electromagnetically heated by induction coil to 1,350 o C and held at temperature for ninety minutes to distill off the adhering salts. The distilled salt vapor rises through a 10 cm diameter throat and condenses inside the cool condenser volume above the crucible assembly. Condensation of the salt vapor in the cool condenser region creates a pressure drop which draws more vapor. During this distilling operation, the steel container prevents the reactive chlorides from contacting the crucible wall, after which it is sacrificed as part of the consolidated waste form. For the consolidation, the temperature is increased to 1,630 o C and held there for three hours. In the top condenser assembly, the condensed salt is frozen into individual wedges formed by removable stainless steel fins which fit the annular space. After several runs, the condenser assembly is opened to remove the salt wedges, which are recycled back into the electrorefiner. 185
8.5.2 Ceramic Waste Form Most of the fission products other than noble metals accumulate in the salt phase, including alkaline metal (Cs and Rb), alkaline earth (Sr and Ba), halide (Br and I), and rare earth (Y, Sm and Eu). These fission products are immobilized in zeolite, a material that adsorbs the fission products in a manner that immobilizes them. The fission product cations in the salt are adsorbed onto the zeolite by ion exchange and a portion of the salt is occluded—that is, it enters molecular cages that trap it in the zeolite structure. Both the adsorbed ions and occluded salt are very resistant to leaching by water. To further improve the leaching resistance, the saltloaded zeolite is consolidated into a monolithic form by combining it with borosilicate glass as binder and sintering it at high temperature. At high temperature, the zeolite is converted to sodalite, a stable naturally occurring mineral. The conversion from zeolite to sodalite can be avoided if the temperature and the time at temperature can be carefully controlled; however this would be difficult for large-scale waste processing operations. In any case, sodalite is preferred for salt retention. Zeolite has larger molecular cages to occlude salt molecule. Sodalite‘s smaller size cages provide better containment of the salt as they inhibit release of the occluded salt molecules. Figure 8-13 illustrates the molecular structures of zeolite and sodalite. Figure 8-13 Molecular structure of zeolite and sodalite In the EBR-II spent fuel treatment, the bond sodium is oxidized into NaCl in the electrolyte. Buildup of NaCl in the electrolyte salt will raise the melting temperature of the salt, so its buildup is limited to approximately 6 wt%. At this point portions of the salt are then treated for disposal. Commercially available zeolite powder contains as much as 22 wt% moisture, which is dried by heating to less than 1 wt% moisture. The disposed salt is crushed to appropriate particle size and then combined with zeolite powder in a V-mixer, heated to 500 o C for approximately 15 hours to allow salt occlusion into the zeolite structure and mixed with 25 wt% glass. 186
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PLENTIFUL ENERGY The Story of the I
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Copyright © 2011 Charles E. Till a
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CONTENTS FOREWORD .................
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CHAPTER 10 APPLICATION OF PYROPROCE
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FOREWORD On a breezy December day i
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CHAPTER 1 ARGONNE NATIONAL LABORATO
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even now is straining the limits of
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with events and time. Till saw the
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it, I saw how a national laboratory
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Figure 1-2. West stands of the Stag
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development of nuclear power for ci
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depended on U.S. ability to maintai
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construction funding kept increasin
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faced a nightmarish combination of
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concept in the next decade.) In sti
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was based on EBR-I experience, but
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Figure 1-9. Experimental Breeder Re
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Figure 1-11. Rendering of the EBR-I
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performance. But the decision had b
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its shakedown in early years it jus
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sense primarily a commercial power
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without electrical generation, the
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Its purpose was to demonstrate the
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of each period, which the managemen
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CHAPTER 2 THE INTEGRAL FAST REACTOR
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A line had been pursued that the re
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The IFR refining process also produ
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director of Argonne a year or two b
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eporting on nuclear power developme
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A few weeks later, the mid-term ele
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2.6 Summary In late 1983, the line
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Argonne would be. My Ph.D. at Imper
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I had worked at the United Kingdom
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hadn‘t bothered us with it. But t
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But I had gone over and over the on
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laboratories.‖ Incidentally, late
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Argonne by this time was one of sev
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3.1.2 Life at the Laboratory in the
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An anecdote: In the cooperative arr
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Cycle Facility‖ went. We pushed i
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(LMFBR), which assumed a very rapid
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the pool was a settled issue; it wa
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During the early stage of the IFR p
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scientific work, not on non-essenti
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e generally held, even as facts inc
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cf per day from Canada via pipeline
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serious, and it is made more seriou
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global economy. The LWR, and the Ad
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supply 11%, and one, the world‘s
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Fatih Birol, has recently been quot
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gas production of little use in the
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expenditures during a decade starti
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thousand tonnes in one large increm
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But the principal line of developme
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Tar sands and oil shale recovery ar
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14. W. H. Ziegler, C. J. Campbell,
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Argonne had been a part of the deve
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Breaches or holes in the fuel cladd
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waste. For efficiency in uranium us
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Further, as a metal, sodium does no
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to the boundaries and many leak fro
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is debatable, it remains our belief
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CHAPTER 6 IFR FUEL CHARACTERISTICS,
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To do this, an extraordinarily simp
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Further cementing the decision was
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the AEC, but the reactor operation
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hands-on access needed to accomplis
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temperature. However, a very substa
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It turned out that the high-plutoni
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In the column ―Pu content % heavy
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40 start-ups and shutdowns 5 15% ov
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During casting, a partial vacuum (1
Page 146 and 147: is in fact a new fuel. Plutonium-ba
Page 148 and 149: 8. G. L. Hofman and L. C. Walters,
Page 150 and 151: characteristics necessary for this.
Page 152 and 153: exchangers, and the steam generator
Page 154 and 155: experiments, as mentioned; this has
Page 156 and 157: sufficient to allow radioactive rel
Page 158 and 159: In the IFR, this loss of the coolin
Page 160 and 161: Figure7- 2. Reactor outlet temperat
Page 162 and 163: for thermal expansion of heavy stru
Page 164 and 165: power to shut down power is basical
Page 166 and 167: criticality. The debris is in the f
Page 168 and 169: 7.10.2 The EBR-I Partial Meltdown T
Page 170 and 171: 7.11 Licensing Implications What ar
Page 172 and 173: The sodium flowing into the steam g
Page 174 and 175: [15] Provisions are also made to co
Page 176 and 177: disassembly comes, it is with a rea
Page 178 and 179: CHAPTER 8 THE PYROPROCESS In the ne
Page 180 and 181: EBR-II purposes, and it established
Page 182 and 183: valuable fuel constituents, uranium
Page 184 and 185: and materials and it had been renam
Page 186 and 187: The first operation is done in the
Page 188 and 189: into the receiver crucible. The hea
Page 190 and 191: In the final step, the pins are arr
Page 192 and 193: Spent Fuel Processed, kg effective
Page 194 and 195: products, highly radioactive and se
Page 198 and 199: If the bond sodium along with the s
Page 200 and 201: CHAPTER 9 THE BASIS OF THE ELECTROR
Page 202 and 203: Whether or not a given reaction can
Page 204 and 205: 9.3 Kinetics of the Reactions Chemi
Page 206 and 207: The exponential exp((E f -E b )/RT)
Page 208 and 209: The electrorefining process brings
Page 210 and 211: cathode operation. Once the solutio
Page 212 and 213: Table 9-2. Measured data and calcul
Page 214 and 215: All four measurements show that eve
Page 216 and 217: The free energy of the reaction of
Page 218 and 219: 2. At an actinide chloride ratio of
Page 220 and 221: CHAPTER 10 APPLICATION OF PYROPROCE
Page 222 and 223: 10.2 Electrolytic Reduction Step 10
Page 224 and 225: The pyrochemical process simply sup
Page 226 and 227: Figure 10-1. Electrolytic reduction
Page 228 and 229: The distribution of fuel constituen
Page 230 and 231: an electrorefiner with a 5001,000 k
Page 232 and 233: aqueous reprocessing plant. The eco
Page 234 and 235: Li metal at the cathode. Lithium me
Page 236 and 237: 4. D. W. Dees and J. P. Ackerman,
Page 238 and 239: Our intent for the IFR technology w
Page 240 and 241: dose to any member of the public mu
Page 242 and 243: IFR process, as we shall see, does
Page 244 and 245: Relative Radiological Toxicity uran
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doses from Tc-99 and I-129 equilibr
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Fraction of Initial Actinide, % pro
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long-lived fission products and tra
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to decay to the point where they co
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References 1. ―Nuclear Waste Poli
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12.1 Introduction Assessment of a p
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History provides empirical evidence
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program offered nations help with n
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Other nations are recycling their s
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uranium-233 cycle has been half-hea
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electrorefiner salt. And this, of c
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those concentrations in making the
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chance of ―pre-ignition‖ leadin
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It is now known that the plutonium
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12.8 Monitoring of Processes Always
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[18] In it he shows that with a spo
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Such a system tracks the quantity a
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weapons grade plutonium. Levels of
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12.13 Summary In IFR technology the
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12. T. P. McLaughlin, et al., ―A
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The earliest fast reactors designed
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India, too, has successfully operat
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levels, actually higher than the di
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for the backend of the fuel cycle,
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$/lb Uranium Price, $/lb U3O8 the f
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the once-through fuel cycle. Howeve
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$/kg 1200 1000 $1000/kg Rep Cost Pu
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Table 13-7. Summary Comparison of F
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fabrication. This, along with a low
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Fissile Cost, $/gm-fissile Fuel Cyc
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13.6 System Aspects The previous se
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waste streams have no long-term dec
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5. S. C. Chetal, ―India‘s Fast
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capacity over this century, in a sy
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thermal properties of NaK—the boi
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It is suspected that the lead corro
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Neutron Yield, Eta Value A = number
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to maintain a hard spectrum, the fu
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Table 14-3. Effects of fuel pin dia
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Fuel Volume Fraction have a large e
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neutron leakages from the core are
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like breeding, does increase such d
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substantial advantage to start with
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Doubling Time, yrs the reactivity c
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14.7 Worldwide Fast Reactor Experie
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limit to its life. The ingenuity of
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Nuclear Capacity, GWe the replaceme
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14.9 How to Deploy Pyroprocessing P
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construction projects. They may see
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inferior to sodium in their thermal
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5. Federation of American Scientist
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Supporting the reactor design and c
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ACKNOWLEDGEMENTS In beginning this
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APPENDIX A DETAILED EXPLANATION OF
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The actinide metals (uranium, pluto
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As noted above, the interactions ri
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3. Equilibrium coefficients give th
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ion is created at the anode. Bulk t
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proceed spontaneously. If the magni
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product chlorides are highly stable
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increases with increasing temperatu
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Equilibrium in a chemical system is
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Exp(-ΔG o /RT) = [ U / Pu ] [ U /
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―in solution.‖ More Pu added to
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appropriate values are used for the
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A.9.5 The Second Cathode Regime: On
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in the real world. Uranium dendrite
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This is the significant number. The
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For those who are curious, the elec
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of concentration of uranium chlorid
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agreement with the measured ratio w
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eference 7. The important calculati
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as well. The numbers were obtained
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Run3: Plutonium isn’t, Uranium is
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The final actinide chloride ratios
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values of several of the constants
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HCDA HFEF HM HWR HTR IAEA ICRP IEA
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ABOUT THE AUTHORS Dr. CHARLES E. TI
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