PLENTIFUL ENERGY

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IFR process, as we shall see, does just that. It removes or very greatly reduces the source of radiation for times far in the future, and makes the prediction of the containment behavior of a repository meaningful: The time over which containment must be strictly maintained drops into the few-hundred-year range, well within the capability of engineering practice—and even within the capabilities of the practices of millennia ago, as the continued presence today of ancient temples, tombs and cathedrals can testify. 11.3 Radioactive Life of Spent Fuel Light Water Reactor (LWR) spent fuel consists of fission products (elements created by neutrons captured by the uranium and plutonium nuclei that resulted in fission), actinides (elements created by neutron capture in uranium that did not cause fission), and uranium remaining as it was when it went into the reactor. Uranium is the largest fraction by far, representing well over 90 percent of the bulk of spent fuel. Three or four percent of the heavy metal (uranium and plutonium, principally) will have fissioned. Of the hundreds of fission product isotopes that result, most decay rapidly to stable (non-radioactive) isotopes. Two very significant exceptions are Sr-90 and Cs-137, which have twenty-nine and thirty-year half-lives, respectively, and which decay by emitting very energetic gamma rays. They are generally the two fission products of most concern. There are very long-lived fission products also, Tc-99, I-129, and Cs-135, which decay with low energies by the expulsion of low energy beta particles (electrons or positrons), the least damaging of radioactive emissions. As a general guide, the longer the life of the radioactive fission product, the lower the energy is of its radioactive emission. About 1 percent of the heavy metal will have captured a neutron, undergone subsequent decay, and thus have been transmuted into higher actinides (also called transuranic isotopes, or TRU) which will not have fissioned. Typically their halflives are long, some stretching into hundreds of thousands of years. Their decay is often by alpha particle emission and they are an ingestion hazard, even in fairly small amounts. Alpha particles are helium nuclei (two protons and two neutrons), heavy as particles go on the atomic scale, and although their range is short and penetrative ability low, their considerable energy is harmful particularly to internal tissue (the skin is sufficient to block external alpha emitters). Uranium, about 95% of the bulk, does not contribute much to the radiological toxicity of the spent fuel. Uranium isotopes found in nature have extremely long half-lives (4.5x10 9 years for U-238 and 7x10 8 years for U-235), and thus emit relatively little radioactivity. 231
Relative Radiological Toxicity The radiological toxicity of typical LWR spent fuel over the years is shown in Figure 11-1. Radiological toxicity here is a relative measure of the cancer risk if ingested or inhaled, which we have normalized to that of the natural uranium ore. As mined, the ore contains uranium along with daughter products that have accumulated by its slow decay over the millennia. That is the form of uranium in nature, as it is accumulated in deposits and distributed in the earth and water (uranium compounds are soluble) all over the globe. 1000 100 Transuranic Elements (Actinides) 10 1 Natural Uranium Ore 0.1 0.01 Fission Products 0.001 10 100 1,000 10,000 100,000 1,000,000 Years Figure 11-1. Relative radiological toxicity of spent fuel constituents The normalization to the natural uranium ore from which the spent fuel originated is the standard we have chosen. If the radiological toxicity drops below the natural uranium ore level, radioactive nuclear waste presents no greater hazard than the ore had in nature. The radiological toxicity curve that crosses the natural uranium line can then be loosely defined as an effective lifetime of the waste components. The radiological toxicity due to the fission product portion of the waste decays with the thirty-year half-life expected from the dominance of strontium and cesium. It drops below the natural uranium ore level in about three hundred years (ten halflives), and becomes relatively harmless (by two orders of magnitude) in less than a thousand years. On the other hand, the toxicity level associated with the actinide portion stays far above that of natural uranium ore and remains at least three orders of magnitude greater than fission products for hundreds of thousands of years. If 99.9% of actinides are removed from the waste form (see previous chapter), then the radiological toxicity of the remaining 0.1% actinides stays below the natural 232
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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
Page 192 and 193: Spent Fuel Processed, kg effective
Page 194 and 195: products, highly radioactive and se
Page 196 and 197: its own bayonet-style partial inter
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 244 and 245: Relative Radiological Toxicity uran
Page 246 and 247: doses from Tc-99 and I-129 equilibr
Page 248 and 249: Fraction of Initial Actinide, % pro
Page 250 and 251: long-lived fission products and tra
Page 252 and 253: to decay to the point where they co
Page 254 and 255: References 1. ―Nuclear Waste Poli
Page 256 and 257: 12.1 Introduction Assessment of a p
Page 258 and 259: History provides empirical evidence
Page 260 and 261: program offered nations help with n
Page 262 and 263: Other nations are recycling their s
Page 264 and 265: uranium-233 cycle has been half-hea
Page 266 and 267: electrorefiner salt. And this, of c
Page 268 and 269: those concentrations in making the
Page 270 and 271: chance of ―pre-ignition‖ leadin
Page 272 and 273: It is now known that the plutonium
Page 274 and 275: 12.8 Monitoring of Processes Always
Page 276 and 277: [18] In it he shows that with a spo
Page 278 and 279: Such a system tracks the quantity a
Page 280 and 281: weapons grade plutonium. Levels of
Page 282 and 283: 12.13 Summary In IFR technology the
Page 284 and 285: 12. T. P. McLaughlin, et al., ―A
Page 286 and 287: The earliest fast reactors designed
Page 288 and 289: India, too, has successfully operat
Page 290 and 291: 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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