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Exp(-ΔG o /RT) = [ U / Pu ] [ U / Pu ] [ PuCl3 / UCl3 ] [ PuCl3 / UCl3 ], where (4) Pu and U are the two elements we are interested in, = activity coefficient, = concentration expressed as mol fraction, ΔG o is the difference between the standard free energies of chloride formation of PuCl 3 and UCl 3, R is the gas constant, 1.987 cal/K, and T is temperature, o K The exponential is calculable from the difference in the free energies of chloride formation of the two metals. The activity coefficients have been measured and are tabulated in the chemical literature, and the ratio of the concentrations of uranium and plutonium chlorides in the salt is measurable, so the ratio of plutonium to uranium in the cadmium to be expected—the number we want—can be calculated. Also very important is how well the fission products are separated from the actinide product. The degree of separation of the waste from the product quantifies the success of this portion of the process. Separation factors measuring the degree of separation of many of the important fission products from uranium product have been measured. [3] Such separation factors are defined first in terms of a distribution coefficient, D, for the individual element. Using the important fission product cesium as an example, the distribution coefficient is the ratio of the cesium in the electrolyte (as cesium chloride, of course) to cesium in the metallic product. (A successful separation will have a very small cesium concentration in the metallic product, for example.) Then the ratio of its distribution to the distribution coefficient of uranium, defined similarly, gives the separation coefficient for cesium with respect to uranium separation. (Strictly, corrections for valences may be necessary in some cases. That need not concern us here, where we need only the principles involved.) D cs = concentration of cesium chloride/ concentration of cesium metal, and with a similar definition for other elements, notably uranium, for which we get: The separation factor of cesium with respect to uranium: SF cs/u = D cs /D u . The separation factors tell us how clean the separations will be. Their basis, once again, is the difference in free energies of formation of the chlorides of the various elements relative to that of uranium. Some measured separation factors are given in Table A-2, taken from Ackerman and Johnson. [3] The values vary from separation factors of 43.1 to 1.6x10 9 for the listed fission products, and from 1.88 to 3.52 for the higher actinides. These are perfectly adequate fission product separations for IFR fuel, whereas for the actinides, small 361
separations between plutonium and both uranium and the actinide above plutonium assure the desirable (for safeguarding purposes) imperfect actinide separations. Table A-2. Separation Factors Relative to Uranium in LiCl –KCl Salt at 775K U 1 Pu 1.88 Np 2.12 Am 3.08 Cm 3.52 Pr 43.1 Nd 44.0 Ce 49 La 130 Gd 150 Dy 500 Y 6000 Sm, Eu, Li, Ba, Sr >10 10 A.9 Actinide Saturation in Liquid Cadmium: A Key to Enhanced Plutonium Depositions Saturation of the liquid cadmium can play a role in the effective operation of a liquid cadmium cathode. With it comes the ability to control, within limits, the possible composition and amount of the actinide product. [4] A.9.1 Solution, Solubility and Saturation A ―solution‖ is defined very precisely to mean a ―solute‖ (in our case uranium or the plutonium-cadmium compound PuCd 6 ) dissolved in a ―solvent‖ (in our case, liquid cadmium). A solution is one uniform homogeneous phase; the solute is dissolved, and there is no solid in solution. (Think of sugar in water; up to the solubility limit, sugar dissolves and the water is still clear: only one phase is there. Beyond the limit, the solution is no longer clear; there is another phase, sugar sludge probably, in it.) If a solution is saturated, no more solute can go ―into solution.‖ Saturated means exactly that, no more and no less: no more solute ―in solution.‖ More can deposit, but the amount that is ―in solution‖ is fixed and cannot increase any more. More U added to a cathode saturated in U will result in the formation of another phase; ―pure‖ metallic U will deposit and it won‘t be dissolved 362
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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
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is in fact a new fuel. Plutonium-ba
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8. G. L. Hofman and L. C. Walters,
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characteristics necessary for this.
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exchangers, and the steam generator
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experiments, as mentioned; this has
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sufficient to allow radioactive rel
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In the IFR, this loss of the coolin
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Figure7- 2. Reactor outlet temperat
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for thermal expansion of heavy stru
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power to shut down power is basical
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criticality. The debris is in the f
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7.10.2 The EBR-I Partial Meltdown T
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7.11 Licensing Implications What ar
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The sodium flowing into the steam g
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[15] Provisions are also made to co
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disassembly comes, it is with a rea
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CHAPTER 8 THE PYROPROCESS In the ne
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EBR-II purposes, and it established
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valuable fuel constituents, uranium
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and materials and it had been renam
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The first operation is done in the
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into the receiver crucible. The hea
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In the final step, the pins are arr
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Spent Fuel Processed, kg effective
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products, highly radioactive and se
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its own bayonet-style partial inter
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If the bond sodium along with the s
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CHAPTER 9 THE BASIS OF THE ELECTROR
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Whether or not a given reaction can
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9.3 Kinetics of the Reactions Chemi
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The exponential exp((E f -E b )/RT)
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The electrorefining process brings
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cathode operation. Once the solutio
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Table 9-2. Measured data and calcul
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All four measurements show that eve
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The free energy of the reaction of
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2. At an actinide chloride ratio of
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CHAPTER 10 APPLICATION OF PYROPROCE
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10.2 Electrolytic Reduction Step 10
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The pyrochemical process simply sup
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Figure 10-1. Electrolytic reduction
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The distribution of fuel constituen
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an electrorefiner with a 5001,000 k
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aqueous reprocessing plant. The eco
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Li metal at the cathode. Lithium me
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4. D. W. Dees and J. P. Ackerman,
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Our intent for the IFR technology w
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dose to any member of the public mu
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IFR process, as we shall see, does
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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
Page 322 and 323: Table 14-3. Effects of fuel pin dia
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Page 342 and 343: construction projects. They may see
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Page 346: 5. Federation of American Scientist
Page 349 and 350: Supporting the reactor design and c
Page 352 and 353: ACKNOWLEDGEMENTS In beginning this
Page 354 and 355: APPENDIX A DETAILED EXPLANATION OF
Page 356 and 357: The actinide metals (uranium, pluto
Page 358 and 359: As noted above, the interactions ri
Page 360 and 361: 3. Equilibrium coefficients give th
Page 362 and 363: ion is created at the anode. Bulk t
Page 364 and 365: proceed spontaneously. If the magni
Page 366 and 367: product chlorides are highly stable
Page 368 and 369: increases with increasing temperatu
Page 370 and 371: Equilibrium in a chemical system is
Page 374 and 375: ―in solution.‖ More Pu added to
Page 376 and 377: appropriate values are used for the
Page 378 and 379: A.9.5 The Second Cathode Regime: On
Page 380 and 381: in the real world. Uranium dendrite
Page 382 and 383: This is the significant number. The
Page 384 and 385: For those who are curious, the elec
Page 386 and 387: of concentration of uranium chlorid
Page 388 and 389: agreement with the measured ratio w
Page 390 and 391: eference 7. The important calculati
Page 392 and 393: as well. The numbers were obtained
Page 394 and 395: Run3: Plutonium isn’t, Uranium is
Page 396 and 397: The final actinide chloride ratios
Page 398: values of several of the constants
Page 401 and 402: HCDA HFEF HM HWR HTR IAEA ICRP IEA
Page 404: ABOUT THE AUTHORS Dr. CHARLES E. TI
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