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The final actinide chloride ratios in the salt ranged downward from 5.66 to 3.31 to 2.86 in the three runs, which are to be compared to 4.1, the calculated ratio PuCl 3 /UCl 3 at equilibrium with both plutonium and uranium saturated in the cadmium. In Run 1, plutonium was saturated, uranium was not; in Run 2, both were saturated, and in Run 3, plutonium was not saturated, uranium was. Where amounts greater than saturation amounts were present in the product, the amounts in grams of the metallic phases are listed in Table A-7. The measured results are compared to calculation by our simple equilibrium expressions in Table A-9 below. Table A-9. Calculated vs. Measured Pu/U Product Ratio Each ratio of actinide chlorides will give the concentration ratio of uranium and plutonium in the cadmium relevant to it up to the point of saturation of one of the actinides. For a PuCl 3 /UCl 3 concentration ratio of 4.1 in the salt, everything is in equilibrium and the ratio of plutonium to uranium in the cathode will be 1.55. For actinide chloride concentration ratios above and below 4.1, the U/Pu ratio in the cadmium will follow the relationships given by the equilibrium coefficient expressions. The degree of agreement between the measurements and our calculations based on equilibrium is gratifying. Run 1 The PuCl 3 /UCl 3 ratio of 5.7 is above the equilibrium ratio of 4.1, and the system will try to equilibrate by subtracting uranium from the cathode to increase the UCl 3 in the electrolyte and bring the PuCl 3 /UCl 3 ratio down. Less uranium than calculated based on the PuCl 3 /UCl 3 ratio of 5.7 was found in the product. Run 2 Initial Actinide Chloride Ratio Final Actinide Chloride Ratio Measured Pu/U Product ratio Calculated in-solution Calculated total Run 1 10.2 5.7 3.0 2.2 2.25 Run 2 5.1 3.3 1.6 1.6 1.6 Run 3 3.7 2.9 0.6 1.1 0.75 Run 4 3.5 2.9 0.7 1.1 0.78 The PuCl 3 /UCl 3 ratio of 3.32 is somewhat below the equilibrium ratio of 4.1. The amounts are both are slightly in excess of saturation. The actinide ratio in the salt now is less than the equilibrium ratio of 4.1, and some of the deposited plutonium would be expected to migrate back into the salt as the system tries to equilibrate. 385
However, the ratio of plutonium to uranium in the deposit does agree with that calculated based on the PuCl 3 /UCl 3 ratio of 3.32. Run 3 The PuCl 3 /UCl 3 ratio of 2.86 is further below the equilibrium ratio. The system will try to add plutonium from the cathode to add PuCl 3 to the electrolyte, reducing the amount of plutonium in the cathode. Here, less plutonium than calculated based on the PuCl 3 /UCl 3 ratio 2.87 was found in the product. Run 4 The PuCl 3 /UCl 3 ratio of 2.85 is essentially the same as in Run 3. The results are the same as well, to the accuracy of calculation and measurement. The run provides assurance of the consistency of results but no new information. All four measurements show that even with high plutonium to uranium ratios in the salt, the plutonium to uranium ratio in the product will be much lower, by a factor varying but in the range of the 2.65 previously calculated for lowering of the product Pu/U ratio from the equilibrium PuCl 3 /UCl 3 ratio of 4.1 in the salt. In other words, getting close to a pure plutonium product without accompanying uranium is extremely difficult, and the presence of actinides above plutonium makes a pure plutonium product impossible. The measurements show that a perfectly adequate plutonium enrichment of the product for reactor fuel recycle is possible with reasonable PuCl 3 /UCl 3 ratios in the salt. The calculations show that the equilibrium assumption allows prediction of the results of these very significant experiments surprisingly well. In summary, we now have the means to estimate the ratio of Pu/U in the product as a function of the PuCl 3 /UCl 3 ratio in the electrolyte salt. At equilibrium with both uranium and plutonium saturated in the cadmium, the ratio of Pu/U product is 1.55. The PuCl 3 /UCl 3 ratio of Run 2 (3.32) is nearest to the calculated equilibrium value of 4.1. It gave both a measured and a calculated value of the Pu/U ratio of 1.6, agreement that is certainly fortuitous, but is gratifying in any case. The conclusion to be drawn overall is that the important Pu/U ratio can be predicted with useful accuracy from these simple considerations and very simple expressions. Neither calculation nor the experiment can be taken to be highly accurate. Many approximations were made in these simple calculations. The assumption of linearity in activities prior to saturation, the assumption of equilibrium or near- equilibrium, the rough corrections for saturation effects; all these and more are relevant. The 386
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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
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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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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 372 and 373: Exp(-ΔG o /RT) = [ U / Pu ] [ U /
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 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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