o i - IEEWH I ANP “”Ttfifligm REQ qi-:b 3 4456 03L098L O Reactors-Aircraft Nuclear Propulsion Sys AEC RESEARGH AND DEVELOPMENT REPORT ) . ... . A THEORETICAL STUDY OF Xe '35 POISONING KINETICS IN FLUID-FUELED, GAS-SPARGED NUCLEAR REACTORS CENTRAL RESEARCH LIBRARY DOCUMENT COLLECTION LIBRARY LOAN COPY DO NOT TRANSFER TO ANOTHER PERSON If you wish someone else to see this document, send in name with document and the library will E M. T. Robinsen 2 "-\ m : e Prfl fi(‘!"?" % CLassirrcamon Muanas . _H“““___ na¥ u._‘?.;_']_c?f__ N KE.?TJ;}'T- f g . e, L OAK RIDGE NATIONAL LABORATORY OPERATED BY UNION CARBIDE NUCLEAR COMPANY A Division of Union Carbide and Carbon Corporation POST OFFICE BOX P * OAK RIDGE, TENNESSEE i ANP Authorization Required ORNL.1924 This document consists of 29 pages. Copy‘fl 220 copies. Series A, Contract No, W-7405-eng-246 SOLID STATE DIVISION A THEORETICAL STUDY OF Xe'35 POISONING KINETICS IN FLUID-FUELED, GAS-SPARGED NUCLEAR REACTORS M. T. Robinson DATE ISSUED OAK RIDGE NATIONAL LABORATORY Operated by UNION CARBIDE NUCLEAR COMPANY A Division of Union Carbide and Carbon Corporation Post Office Box P Oak Ridge, Tennessee i T 4450 D3Lga,, . VPN A WN MUY AL MANEDECPOQOEROCDPENEIZOOONMANIOCDNONR * ANP AUTHORIZATION REQUIRED #PRNL-1924 Reactors-Aircrff:Nuclear Propulsion Systems HB679 (17th ed.) 5 § AR AN YR INTERNAL DISTRIBUTION 0 ’ . G. Affel 45. DFFE. Ferguson . R. Baldock ‘:"“ 46._;'} f. P. Fraas . J. Barton R H. Frye, Jr. D. Baumann ): W, T. Furgerson . G. Berggren #4¥. J. L. Gabbard O. Betterton, Jr. i . 4#0. H. C. Gray S. Billington k- 4851, R. J. Gray Binder e ’#} 52. W.R. Grimes . F. Blankenship 8 53. W. 0. Harms (consultant) . H. Blewitt ¥ 54. C.S. Harrill P. Blizard A 4 55. E. E. Hoffman D. Bopp 56. A. Hollaender . J. Borkowski 57. D. K. Holmes . E. Boyd 58. A. S. Householder . A, Bredig 59. J. T. Howe . Brooks (consultant) 60. L. K. Jetter E. Browning 61. R. J. Jones R. Bruce 62. W. H. Jordan E. Brundage 63. G. W. 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AR ) Chicago F’ufé‘ roup Chief of Navalf@esearch _ Convair-General@ynamics Corglbration Director of Labofigories (WC Director of Requ|lments (AJDRQ) Director of Resecih and D@felopment (AFDRD-ANP) Directorate of Sysffins Maglfgement (RDZ-ISN) Directorate of Sy:\\'\ s -J,“ hgement (RDZ-1SS) Equipment Labord;f pC) General Electric Ga\ibadll (ANPD) Hartford Area OfficdW Headquarters, Air ol Special Weapons Center lLockland Area Officidlll Los Alamos Scientif; Materials Laborat"' d s Office (WADC) National Advisory#F#i#ilktee for Aeronautics, Cleveland National Advisogiiilfo | ee for Aeronautics, Washington North Americanp - c. (Aerophysics Division) Nuclear Develcjililént Cofjikation Patent Branch shingf' B Power Plant |i#lbratory (WEDC) Pratt and Wh Aircraft EilRision (Fox Project) Sandia Corp#iilfion “‘. | School of , ion '\Aedicine\;-'\}1 ! USAF ProjlfRand 4 University§ Wright Aig Technicaf S aboratory n l.aboratory, Livermore COSI-3) Ridge ent, AEC, ORO alifornia Radidl velopment Centel§ formation Service, 3 Division #ilResearch and Deve} — . 0 ® N O bW _r Ca0 CONTENTS FEPOAUETION oottt ettt e et ettt e s et s ettt et r b e s shen st s ] Derivation of the Differential EQuations ............oocoii i e 1 Relations Between the Various Phase-Transfer Rate Constants.............ccooveiiiiiiiiiiine, 4 Solution of the Differential EQUAtions ...........cooooiiiiiii e e, 6 Steady-State Operation of @ Reactor...........cocoiiiiiiiiiiiiciiiceecc e s 9 Kinetics of Xe 32 Poisoning inthe ARE ... e 12 Kinetics of Xe '3 Poisoning in the ART ..o 15 Kinetics of Xe'3% Poisoning During Shutdowns.........coco.ooviiiiiiece e, 18 Nomograms for Xenon-Poisoning Caleulations ...........cocooiiii 18 A THEORETICAL STUDY OF Xe '35 POISONING KINETICS IN FLUID-FUELED, GAS-SPARGED NUCLEAR REACTORS M. T. Robinson 1. INTRODUCTION One of the substantial advantages claimed for liquid fuels in very-high-power nuclear reactors is the easy removal of Xe'3® from the fuel, with the consequent gains in neutron economy.' This claim is at least partly supported by operating experience with the ARE,?2 This report is 135 boisoning in a reactor in which this concerned with a theoretical study of the kinetics of Xe volatile poison is continuously removed by a stream of sparging gas. The theory is applied to the experience with the ARE and is used to make predictions for the ART. Some comments on full-scale aircraft power plants are also included. The system is assumed to consist of two phases: the liquid fuel and the sparging gas. The theory is concerned only with volume-averaged concentrations and neutron fluxes. Turbulent motion of the two fluids is held to assure thorough mixing within each phase. The appropriate differential equations which describe the behavior of the poisoning in such a system are derived and solved. Steady-state behavior during high-power operation of the reactor is discussed. Detailed kinetics of the poisoning during the approach to steady state are studied through a series of calculations performed on the Oracle. A brief discussion of shutdown behavior follows, 135 A final section presents a rapid approximate method for calculating Xe poisoning in gas- sparged fluid-fueled reactors. 2. DERIVATION OF THE DIFFERENTIAL EQUATIONS 135 The volume-averaged concentration of Xe in the fuel of a fluid-fueled nuclear reactor changes because of a number of different processes, as shown schematically in Fig. 1. These ]W. R. Grimes et al., The Reactor Handbook, vol 2 (September 1953), p 973. 2M. T. Robinson, W. A, Brooksbank, and D. E. Guss, ANP Quar, Prog. Rep, Dec, 10, 1954, ORNL- 1816, p 124-125. L ] SSD-A-1167 ORNL—-LR~DWG 6430A PROCUCTION FROM 135 DECAY OF I LOSS BY FLOW OF TRANSFER OF xe'33 ‘ LOSS BY GAS FROM SYSTEM NRLLIY LIQUID TO GAS xe'33 N THERMAL-NEUTRON ABSORPTION SPARGING - GAS y35 | LIQUID-FUEL o LOSS BY PHASE TRANSFER OF Xe PHASE o RADIOACT IVE DECAY GAS TO LIQUID * LOSS BY RADIOACTIVE DECAY DIRECT PRODUCT!ION IN FISSION Fig. 1. Processes Governing Xe 133 Poisoning in Fluid-Fueled Reactors. C e ‘:‘; A processes are as follows (see Table 1 for definitions of all symbols used): 1. direct production from fission, Rate 1 = yxefifgfi ; (2.1) 2. production from decay of 1133, -aat Rate 2 = ylzfgb(] - e ) ; (2.2) 3. transfer from the gas phase to the liquid phase, AegVe Rate 3 = ——— (2.3) VL TABLE 1. DEFINITION OF SYMBOLS English Greek Lefl.ers Definifion Leflers Defin”ion A Area of liquid-gas boundary surface % 100yxeaf/au ag Activity of Xe'33 in the gas phase a, 100y|0’f/0'u a, Activity of Xe '35 in the liquid phase a, )\Ir/,B)\J’r = RTS; see Eq. 3.4 cc Concentration of Xe '35 in gas phase a, Radioactive decay constant of 1133 c, Concentration of Xe '35 in liquid a, Radioactive decay constant of Xe!3% phase A V, Ve &0 Concentration of 1'3% at ¢ = 0; see 135 Eq. 4.18 "1 Fission yield of | T . 135 k* Mass-transfer film coefficient Yxe Fission yield of Xe L o+ A+ A )\f Rate constant for transfer of xenon ! 4 / L from liquid to gas k, a, + a2[3)\1r + Ag )\g vG/VG b Partial pressure of Xe'!3> in gas phase A Txe® 0’ Rote of mass transfer A, Rate constant for transfer of xenon from gas to liquid R Universal gas constant AgE 2 O'f Microscopic fission cross section s Solubility coefficient of xenon in fuel of U233 T Absolute temperature Ef Macroscopic fission cross section of fuel t Time . ) T, Microscopic neutron absorption cross Ve Volumetric flow rate of sparging gas section of U235 Ve Volume of gas phase 2, Macroscopic neutron absorption cross v, Volume of liquid phase section of fuel . Xe 135 poisoning in fuel Oye Microscopic neutron absorption cross . 135 section of Xe y “Equivalent poisoning” in gas phase; see Eq. 2.14 b Volume-averaged thermal-neutron flux 4, loss by radioactive decay, . Rate 4 = —oc, (2.4) 5. loss by absorption of thermal neutrons, Rate 5 = Ty PC, (2.5) 6. loss by transfer to the gas phase, Rate 6 = —)\ch . (2.6) 135 The over-all time dependence of the Xe concentration in the liquid phase is given by the sum of these six rates: VG . -t L= Vbt yE el - e ) +.7'L_A’CG - oy ogd + Adey . 27) 135 The processes which change the volume-averaged Xe '*” concentration in the gas phase are as follows: 7. transfer from the liquid phase, t\chVL Rate 7 = —— (2.8) VG 8. loss by radioactive decay, Rate 8 = ~AyC o ; (2.9) 9. loss by transfer to the liquid phase, Rate 9 = -A c. ; (2.10) 10. loss by flow of gas out of the reactor, Yc‘G Rate 10 = ~ v (2.11) 135 Several ways in which changes might occur in the concentration of Xe in the gas phase have been specifically neglected; these are: 11. loss by absorption of thermal neutrons; 12. production from decay of 1'33 or from fission. This implies the neglect of transfer processes (like 3, 7, 9, and 10) involving 1'3% or U235, 135 The over-all time dependence of the Xe concentration in the gas phase is given by the sum of processes 7 through 10 to be . Vi ( Vs Cc = A c, = |ay + A+ — e - (2.12) Ve / TV, 135 In this discussion of the behavior of a nuclear reactor, the behavior of the Xe poisoning is of primary interest and is defined as 1000y, ¢, 2.1 X = ————Eu . . The related quantity y is defined as ]OG'TXQCG .14 Yy = s . . U The virtue of this latter quantity stems from the identity X CL o (2.15) y €c which will be required in deriving a relationship between )\/ and A. By the use of Eqgs. 2.7, 2.12, 2.13, and 2.14 and some abbreviations from Table 1, the differential equations for the poisoning are written as . —ant s o= oagh, +ad (1~ e 3) 4oy — (g + A+ A x (2.16) y = BAx = (ag + a;BA, + Ay . (2.17) The above equations apply during the nuclear power operation of a reactor. However, the behavior of the poisoning during a shutdown must also be discussed. Inthis case it is necessary to set A, = 0 and to replace the first two terms of Eq. 2.16 by the source term agdge 3. (2.18) The boundary conditions needed in solving Eqs. 2.16 and 2.17 are discussed in Sec. 4. 3. RELATIONS BETWEEN THE VARIOUS PHASE-TRANSFER RATE CONSTANTS The problem of studying the kinetics of Xe!33 poisoning can be simplified by eliminating one of the phase-transfer rate constants, defined in Egs. 2.6 and 2.10, The total rate of transfer of xenon from the liquid phase to the gas phase is )\/VLCL. The total rate of transfer in the reverse direction is AV c . Now, while it probably cannot be realized in practice, there exists some pair of values (c’&, cz) corresponding to true thermodynamic equilibrium between the two phases. The “‘law of mass action'’® requires that under these conditions the amount of material entering a phase be the same as the amount leaving, that is, that ,\vac}: - )\'VGc*(‘; or VL CE, A= A — — (3.1) VG e 3C. M. Guldberg and P, Waage, Etudes sur les affinities chimiques, 1867, The solubility coefficient of a gas in a liquid is the equilibrium concentration of solute in the liquid phase when the partial pressure of the substance in the gas phase is 1 atm. That is, c* = prS = cX RTS , (3.2) where the ideal gas law has been used in the form b = g RT 135 to relate the Xe pressure to its concentration in the gas phase. A combination of Egs. 2.1 and 3.2 gives the desired result: vV L A= A, RTS — . r f VG ’ (3 3) whence a, = RTS . (3.4) Thus equilibrium solubility data may be used to eliminate the rate constant A Also, a relation may be derived between the ‘‘true’’ rate constants, z\f and A, and the *‘ap- parent’’ rate constant,? :\P. The latter is defined by Net Xe '3% transfer rate = -z\ch . (3.5) Equating this to the sum of rates defined in Egs. 2.3 and 2.6, it is found that A, = A - ,\,fi ° (3.6) Vi cp or, introducing Eq. 3.3, c ’\P = Af 1 ~ RTS? . (3.7) If Egs. 3.4 and 2.15 are introduced, then Qyy /\p = A 1 - - . (3.8) Thus experimentally derived values of )\p may be compared with values calculated from the solutions to Eqs. 2.16 and 2.17. The connection of the rate constant )\f to the usual mass-transfer film coefficient may be shown by noting that the total net current of matter across the boundary between the liquid and gas phases is Q"= -NVie, + AVgeg = MV, e, ~ RTS¢g) (3.9) r According to the usual mass-transfer analysis,® the total current may be written as Q" = —k"Ala;, - ag) . (3.10) 4. L. Meem, The Xenon Problem in the ART, ORNL CF-54-5-1 (May 3, 1954). SG. G. Brown et al., Unit Operations, p 510 f, Wiley, New York, 1950. Both phases are assumed to be ideal. The xenon activity in the liquid may be replaced by the concentration. Therefore the standard state in the gas phase must be considered as that pressure of xenon in equilibrium with unit concentration in the liquid. Thus a. = pS = RTSc. . Then Eq. 3.10 becomes Q" = ~k’Alc, - RTSc.) . (3.11) Comparison of Eqs. 3.9 and 3.11 yields k’A (3.12) L In principle, the film coefficient 2" can be computed from the geometry of the system and the physical properties and flow rate of the liquid fuel through a relation of the type k’s = f(SC, Re) , (3.]3) L 135 where s is a characteristic dimension; D, is the diffusion coefficient of Xe in the liquid; Re is the Reynolds number of the liquid; and Sc, the Schmidt number, is given by vy Sec = - I Dy in which v, is the kinematic viscosity of the liquid. It does not appear practical to calculate )\f in this way, because of the complicated geometry and flow regime obtaining in the ARE and ART. 4. SOLUTION OF THE DIFFERENTIAL EQUATIONS 135 The time dependence of the poisoning of a nuclear reactor due to Xe may be expressed by the differential equations x = [ (1) + ahy — kyx (4.1) and y = Bx = kyy . (4.2) The source term is ) = agh, + ap (1 = ¢ %) (4.3) when the reactor is in operation and fole) = aa&oe—aat (4.4) |l35 otherwise. The quantity &0 is related to the amount of present at t = 0, By solving Eq. 4.2 for x, differentiating with respect to t, and combining the results with Eq. 4.1, the differential equation y o+ (kg + k))y + (kiky = aBA)y = B () is obtained. The solution to this equation may be written as --K.IZ y = (I)n(t) + Ae + B_e . where 1 2 2 q =5 by + &y + ik, — 57 + 40,803] ' J Ky = (kg + Ry = Ve - k)2 B2 -~ gt (g + a)BAA, B e D) = i kyky — a BAf (k) — ag)lk, ~ ay) - azfi)\? I B)lfaacfioe (ky = ag)(ky - aj) ~ azfi)‘f Combining these results with Eq. 4.2 yields () = 1 -K]t 2 where (CLO + al)kz)\L a])\L( ®](t) = - kyky = aBAf k) = ag)(ky — a5) — a,BA] ...a.at %&0 (ky ~ azle @z(t) = (k) — a3)lk, - a3) - 2'8)‘? The most general boundary conditions are As t — 0, X —> x, and Yy —>yg - Inserting these conditions into Eas. 4.6 and 4.9, the integration constants become ky = Ky B, A, =——lyg =0, O] - —— {x, -~ 6(0)] and 1 B, = ~——lyy = 9,00 + ———[x, - ©,0) . (4.5) (4.6) (4.7a) (4.7b) (4.8a) (4.9) (4.10a) (4.100) (4.11) (4.12a) (4.125) In this report three special cases will be considered: Case |. Reactor operation starting with "‘clean’’ condition. ~ The poisoning is given by Eq. 4.9, using the function 4.10a. The integration constants are found from Eqs. 4.12a and 5, using x5 = yg = 0 and the quantities (D](O) and ®l(0)' Case |l. Reactor operation at zero nuclear power, after a period of high-power operation. -~ The poisoning is given by Eq. 4.9, using the function 4,106, The initial conditions are found from solutions to the problem of case I. In this instance A, = 0, and the quantity &0 is found from the equation ady = ari (1 - e , (4.13) where A[ is the value of A, for the preceding period of high-power operation and ¢’ is the time of operation. Case lll. Sparging of reactor after a period of complete shutdown, during which no xenon is removed. — The poisoning is given by Eq. 4.9, using the function @,(t). In this case A, =0, Yo = 0, and &0 is found from r’ , (4.14) -a,t’ ~ant a3&0=a/\(]-—-e ) 3 where ¢ ” is the time between the shutdown and the time ¢t = 0. The quantity x, is calculated from rr a A’ » rr »r -a,tl 1L ~al —a.t -a,tl x0=x0e4 +— (T -e 3)e 3 - %) - o ' (4.15) where xg is the poisoning at reactor shutdown, found from the solution to the problem of case . In dealing with cases Il and Il above, it is of interest to know whether or not the quantities x and y reach their extreme values {maxima) at the same time. When x reaches its maximum value, from Eqgs. 4.1 and 4.2, then ky* = BA [ = (kyky = azfi)\?)y* ' (4.16) where the asterisks indicate the special time value. It can readily be shown that the coefficients of /5 and of y* are both always positive quantities. Thus y* can vanish only if BA; y¥ = — 3 (4.17) kik, — azfi)\f Comparison of this equation with Eq. 4.6 shows that Eq. 4.17 cannot be satisfied in general, so that the extreme behavior of x and ¥y cannot be examined by studying the differential equations alone. 5. STEADY-STATE OPERATION OF A REACTOR For very long times of high-power operation, the poisoning reaches a steady-state value, From Eqs. 4.12 and 4.7, the steady-state values of x and y are® (an + a])kz)\L - Tt 5.1) 2 k]kz - azfi)\f and (g + a]))\Lfi)\f B)\f . =— X . (5.2) kiky, ~ azfi)\f 2 These relations can be used in estimating the steady-state poisoning of a reactor under various Yo = conditions. The most convenient way to make these estimates is first to calculate A (OL4 + A) AL 59 a, + )\g + az,B)\f This result is obtained by substituting Eqs. 5.1 and 5.2 into Eq. 3.8. If the mean lives T: = )\% (5.4a) v and ] 7 = (5.45) / are now introduced, then Ty =T +_a4 oy ) (5.54) Since a, << )\g, this expression may be rewritten as RTS v, G Then x__ is computed through the relationship (ao + a]).\L I —— (5.6) an + A+ )\P The data in Table 2 have been used to estimate the steady-state poisoning, x_, in the ART for various assumed values of the phase-transfer mean life. The results are presented in Fig. 2. It is of interest to examine briefly the expected behavior of ART-type reactors of higher power, Although the poisoning of an unsparged reactor of this type is essentially independent 6By an argument similar to that at the end of Sec. 4, it may be shown that x and y do not reach steady- state values simultaneously. Egquations 5.1 and 5.2 apply only after both quantities reach steady state. 10 TABLE 2. DATA FOR NUMERICAL CALCULATION Numerical Data ay = 0.254% R = 82.0567 cc-atm/mole/°K a, = 4.74% T = 1033°K (1400°F) a, = 0.0509 S =6 x 10~7 moles/cc-atm(®) ay = 2.87 x 107% sec™! Oye = 1.7 x 108 barns(®) a, = 2.09 x 1075 sec™! Reactor Data ARE (¢} ART(d) vV, 5.35 f* 5.64 ft* V 1 0.31 #* ve 0.25 cc/sec 1000 STP liters/day @ 8 x 10" neutrons/cm?/sec 1 x 10" neutrons/cm?/sec B 5.35 18.2 A 1.36 x 1076 sec™! 1.7 x 104 sec™! (a)R. F. Newton, personal communication. “’)w. K. Ergen and H. W. Bertini, ANP Quar. Prog. Rep. March 10, 1955, ORNL-1864, p 16. (C)J. L. Meem, personal communication and ARE Nuclear Log Book, ORNL Classified Notebook 4210, (dy, T, Furgerson and J. L., Meem, personal communication. of power, very large increases in poisoning are possible with increased power when efficient sparging is employed. Only the most optimistic case will be considered, with 7= 0. Equation 5.6 may then be written as (ao + a,))\L - : 7 o "X, + (/RIS V,) &7 If there are no major differences in design of such a reactor and in particular if the fuel volume and dilution factor are about the same as in the ART, the poisoning may be estimated on the basis of ART data, by simply adjusting A, in proportion to the power change. The results are presented in Fig. 3.7 TA scale for the amounts of helium required may be visualized by noting that an ordinary cylinder of helium contains 220 scf of gas (6230 liters). !t may also be remarked that if’ff is obout 5 min, requiring 5000 STP liters of helium per day to maintain about 0.5% poisoning in a 300-Mw reactor, and if the aircraft flies ot o speed of 1000 mph (about Mach 1.3 at sea level), the plane will get some 18 miles per gallon of helium. S!!-B-H 68 ORNL-LR-DWG-6434 1.5 1 <10 \\ g \ & \ = 20 min | = S T —— =15 min o - t o "o > 05 \ --—-.__________ rf: 10 rl-nln | \ & *L \"‘"—-—.____ " T, 2 min | \________- rf= 0 nI“n 0 ! 0 1000 2000 3000 4000 5000 SPARGING-GAS FLOW RATE (stp liters/day) Fig. 2. Steady-State Xe!33 Poisoning in the ART as a Function of Sparging-Gas Flow Rate for Various Assumed Values of the Phase-Transfer Mean Life Tpe SSD-B-!!1O ORNL-LR-DWG-7317 PHASE-TRANSFER MEAN LWE,I?'O .Tafl 600 Mw 300 Mw 150 Mw 60 Mw I w s oS Xe'>® POISONING (%) o 05N \\\\ \\\\\\»——-— ~ 0 0 2000 4000 6000 8000 10,000 SPARGING GAS FLOW RATE (STP liters /day) Fig. 3. Steady-State Xe '*° Poisoning in ART-Type Reactors as a Function of Sparging-Gas Flow Rate for Yarious Assumed Reactor Powers. 11 12 Appaangly, other things being equal, the sparging-gas flow rate must increase linearly with power, to maintain constant poisoning. It should be noted that while a decreased fuel volume increases the term [vG/(RTS V)l in Eq. 5.7, this is roughly compensated by a corresponding increase in AL’ which is proportional to the volume-averaged flux. 6. KINETICS OF Xe'35 POISONING IN THE ARE An extensive series of calculations has been performed on the Oracle,® the approach to steady state of the Xe'33 in Figs. 4 through 7. Figure 4 illustrates the dependence of the Xe'® to aid in studying poisoning in the ARE. Typical results are presented 5 poisoning kinetics on the value of ?xf. Note that curves for all values of )tf > 6 x 1073 sec™! fall together on the scale chosen in the 8Coding and supervision of the calculations were done by C, L. Gerberich, ORNL Mathematics Panel, Results were obtained by using Egs. 4.1, 4.2, and 3.8, together with numerical data from Table 2, except as noted in the text. SSD-B-I !'1 ORNL-LR-DWG-T7318 0.09 — A= 210 % sec! 0.08 A =2x10 ! ~ 0.07 & ; 0.06 X, =6 x i0-4 Sec-i = z 3 0.05 A =6 x10°3 sec™ £ 004 " —>°<’ 003 b e 0.25 cc/secs 1 0.02 cxe¢=|‘36 x 10" sec 0.01 0 0 10 20 30 40 50 60 70 80 90 100 " TIME {hr} Fig. 4. Effect of )\/ on Xe '35 Purging in the ARE. 550-B-1Z12 ORNL-LR-DWG-7398 =0 @ =(Q.25 cc/sec =0.50 cc/sec =1.00 cc/sec Ar = 6x10°% sec’! . -6 - :rxe¢-l.36x10 sec 0 10 20 30 40 5 60 70 8 90 100 TIME (hr} Fig. 5. Effect of Sparging-Gas Flow Rate on Xe'33 Poisoning in the ARE. SSD-B- ORNL-LR-DWG-T 399 014 1 :2.80 x10° sec” o n o O o = @ O =1.36 x 105 sec”! < D o o Q B A =6 2104 sec! =(.25 ¢c/sec Xe'>> POISONING (%) o < o Q 70 80 90 100 o 35 20 30 40 5 60 TIME {hr) Fig. 6. Effect of A, on Xe '35 Poisoning in the ARE. SSD-B- 4 ORNL-LR-DWG-T400 A (sec™) ¥, (cc/sec) 6x10* 1.00 6x10': 0.50 -3 ex1d 0.25 10 ex10? 0.00 _ 6x10> 0.25 T 1104 0.25 L 2 .Y 10 0O 10 20 30 40 50 60 70 80 90 100 TIME (hr) Fig. 7. Variation of the Apparent Purge Constant with Time in the ARE. figure. This results from the small volumetric flow rate of off gas in the ARE. This flow rate is rate-determining, making an accurate estimate of )\/ from experimental data difficuit. Figure 5 illustrates the poisoning effects that occur as a result of variations in the sparging- gas flow rate, v, ot a value )Lf = 6 x 1074 sec=!. A comparison of Figs. 3 and 4 shows that at early times (up to 10 hr or so) the rate of Xe 133 removal is primarily governed by the rate of phase transfer, while for longer times the gas flow rate becomes controlling. Thus, under ARE conditions, fission-gas removal may be termed ‘‘off-gas controlled."’ Figure 6 illustrates the effects of A, on poisoning kinetics. As might be anticipated, the results are roughly proportional to A, . Figure 7 presents results on the time dependence of )\p, which is called here the ‘‘apparent rate constant’’ for transfer of Xe'3® from fuel to off gas. The large decrease in )tp with time is clearly evident. Note also that d)tp/dt is everywhere negative. Theory and experiment may be compared as follows.? By employing the abbreviations f6) = agh, + ap, (1 - e ) (6.1a) and gty = ay + A, + )\P(t) , (6.15) the differential equation 2.16 may be written as x(t) = f(t) - gle)x(e) . (6.2) Expanding each of the functions in Eq. 6.2 about the origin, e 2 .l.t3 xot xo x(t) = x4t + e (6.32) . fot? fe) = fo + fot + + e, (6.3b) . g ot glt) = gg + gyt + + e, (6.3c) where the subscript zero represents values at the origin (¢t = 0). If Egs. 6.3z, b, and c are introduced into Eq. 6.2 and if the coefficient of each power of ¢ is equated to zero, then x.‘o = /0 = O.DA.L ’ (6-40) .’;0 = f;a ~ fo8g = (205 — aggoh, (6.4b) This approach was suggested by D. K. Holmes, ORNL Solid State Division. 13 14 xg = fo = fo8g = foB2 + 28g) = ~[a;05 + a5, + (g2 + &N, (6.4c) Now, in principle, a set of experimental data may be fitted to a power series {Eq. 6.3a), and the various coefficients of the series (Eq. 6.3c) can be determined from Eqs. 6.44, b, and c. Note that from Eq. 3.8 AP(O) = )\/ , so that the value of the coefficient g, (i.e., the behavior of the poisoning near the origin) is of primary concern. The experimental data on poisoning in the ARE'? are given in Table 3, along with calculated 149 U235, The neutron capture cross section of Sm'4? 11 contributions due to Sm and to burnup of was taken as 53,000 barns,'! and the burnup effect was calculated from (Ak) 0.232AM k burnup M where % is the infinite multiplication constant and M is the mass of U?33 in the reactor. Other 149 data were taken from Table 2. Since the Sm and burnup contributions are well within the experimental error in the total poisoning, the experimental results are taken to apply to Xe!33 poisoning alone. The results from the ARE cannot be treated by the method described above for two major reasons: 1. The ARE data are based on the assumption that the origin of the (x,?) coordinates was at the start of the experiment. Since about 7 hr of high-power operation preceded the ‘‘xenon 135 experiment,’’ 1% both 1135 and Xe!35 were present in the core at the time “‘zero’’ in Table 3. ARE Nuclear Log Book, ORNL Classified Notebook 4210, ”S. Glasstone and M, C. Edlund, Elements of Nuclear Reactor Theory, p 338, VYan Nostrand, New York, 1952, TABLE 3. EXPERIMENTAL DATA ON ARE POISONING Calculated Poisoning (%) Time Total Poisoning (hr) (%) Burnup 5, 149 xo 135 0 0 0 0 0 1.3 0,003 £ 0,001 0.0001 0.0000 0.004 12,7 0.006 * 0,002 0.0006 0.0003 0.110 13.7 0.009 * 0.002 0.0006 0.0003 0.119 16.0 0.012 £ 0,002 0.0007 0.0004 0.144 20,2 0.015 * 0,003 0.0009 0.0006 0.182 2, Applicatiamatmthe method outlined above requires knowledge of /\L. This quantity governs the scale of the x-coordinate. For the present calculations, a value of 1.36 x 10~¢ sec™! was assumed, based on 1.7 x 10% barns for the Xe!3% cross section and 8 x 101! neutrons/cm?/sec for the ARE thermal flux. 135 cross section in the ARE is nearer 1.4 x 10° It has recently been shown that the Xe barns.'2 The flux value employed was based on the values 575 barns for the U233 fission cross section; 173 Mev per fission absorbed in the reactor; fuel density 3.24 g/cc; composition 13.59 wt % uranium, 93.4% enriched; and 2 Mw reactor power. The resulting value for the flux is not more precise than 120%. It does not appear possible to expect agreement better than about a factor of 2 between theory and experiment. On this basis, results from the ARE have merely been compared with calculated curves similar to those of Fig. 4. It is concluded that )\f must be larger than about 5 x 10~4 sec~! and is probably around 1 x 1073 sec™!. 7. KINETICS OF Xe'35 POISONING IN THE ART In this section the results of Oracle computations of the time dependence of the Xe'3® poisoning in the ART are presented and discussed. The data employed are those of Table 2, except as noted. Typical results are shown in Figs. 8 through 12. 2w, K. Ergen and H. W. Bertini, ANP Quar. Prog. Rep. March 10, 1955, ORNL-1864, p 16. Y A * o S$SD-C-1223 ORNL-LR-DWG-7677 | I l l 1.2 Ar= 6x10% sec! (7,228 min) _ 10 // A,=8x10'4 sec’ {z=21 min) _ - | [ L L [l ] ] Ar=1 x10° se¢! {r,=17 min) ~ 0.8 A s / // o0 206 /// A= 2x10°3 sec? (1,283 min) ] Z /// Fx2x sec ' (1,=8.3 min ® / —— i i i f O . O ng /// // )‘,=4:(10'3 sec ! (r,=42 Imin)—fl n 4 t t T "o » /,/ A= 8x10° sec! (r,=2.4 min)— 0.2 //,/"'—'—f | ] /A/ )~,,=6x10'2 sec’ (r/=0.3min) _| 0 L] oy, =1.70 x10% sec’ xg=4.53n:10'3 sec’’ ’ (,=1030 STP liiters /day) | b 0 20 40 60 80 100 TIME (hr) Fig. 8. Effect of )t/ on Xe 135 Poisoning Kinetics in the ART. 15 16 Yy SSD-B-1222 /o [ T [ ORNL-LR-DWG-7676 ] i ! W o na W ) o \ | \ \ | \ /éz =0 { STEADY*STATE POISONING =3.98 %) | - T4 o UXe¢ =1.70 x10 " sec | T 1 100 ° A=A x 10 ® sec” (_2?20 (lrf-17m1n)l ‘ =z = | ' S ] | | 2 '@ = 510 litersgrp / day X 1.0 / | I ‘ : 05 \l{q = 103i0 liters g1 / day . \ o 10 20 30 40 50 60 70 80 90 TIME (hr) Fig. 9. Effect of Sparging-Gas Flow Rate on ART Poisoning Kinetics. o s SSD-B-1224 ORNL-LR-DWG-7678 1.2 T 7 T | I ! [ v, = C (STEADY-STATE POISONING =3.97 % ) 1.0 ; 208 y, = 260 STP liters / day (29 /’ — 2 06—~ v v, =510 STP liters /day 2 -/ L 8 04 | v, = 1030 STP lifers /day 2 /S ———— /// aXeqb=1.TOx1O sec 0.2 - / Ar =4 x10 " sec ( Tf =4.2 min ) O | ] ! O {0 20 30 40 50 60 TIME (hr) 70 80 90 100 Fig. 10. Effect of Sparging-Gas Flow Rate on ART Poisoning Kinetics. o= -B-1225 ORNL - LR-DWG- SSD-A-1226 _q ORNL- L R-DWG-7680 Ty ®=1.70x10 " sec ¥, =1030 STP liters/day 102 EACH CURVE IS LABELED WITH THE APPROPRIATE VALUE OF X, <1030 STP liters/ day 1 GxTO-Z sec! = 2 _ .- ¥* 510 STP liters/day I ZxICEZ sec_1 I 110" sec 3 %+ 260 STP liters /day K 6xG° sec’ ¥ 4x10° sec’ T o 2x0° sed’ 3 o $=170x10 e T o “(L sec_1 - a o < YO 8xi0° sec - - = o - - § Xy = 4x10 Tsec E X 6!104 seci :q {rp= 4.2 min} R 15t 163 0 10 20 30 40 50 €0 0 10 20 30 TIME (hr} TIME (hr) Fig. 11. Time Dependence of the Apparent Fig. 12, Time Dependence of the Apparent Rate Constant I\.P in the ART. Rate Constant Ap in the ART, Figure 8 illustrates the dependence of poisoning kinetics on the value of )lf, for a value of )\g = 4.53 x 10~3 sec™! (vg = 1030 STP liters/day).!3 The effects of sparging-gas flow rate are presented in Figs. 9 and 10 for two different values of )\./. Because of the much higher sparging-gas flow rates, the ART will not be as insensitive to the rate of phase transfer as was the ARE. Examination of Figs. 9 and 10 shows that the reactor will be more sensitive to off- gas flow rate if )\f is comparatively small than it will if )tf is comparatively large. Poisoning kinetics in the ART can be termed neither ‘‘off-gas controlled’’ nor ‘‘phase-transfer controlled,”’ both processes being appreciably rate determining. The time behavior of the apparent rate constant, )\p, is somewhat different from that in the ARE, because of the much greater sparging-gas flow rate in the ART, Examination of Figs. 11 and 12 shows that at high gas flow rates )\p reaches its steady-state value very rapidly ~ only about 3 hr being required, compared with about 40 hr in the ARE. Physically, this means that the gas phase in the ART reaches a steady state with the fuel phase very rapidly. Recause of the rapid approach to steady state of )\P, it is possible to use the approximate method of Sec. 9 for rapid calculations of ART poisoning kinetics. ]3|n converting the values of A_ to the values of v quoted, it has been assumed that the gas pressure &g in the ART swirl chamber was about 2 psig. Then Ve (STP liters/day) = 2.27 X ]05 Ag (sec_]). 17 18 e 8. KINETICS OF Xe'3® POISONING DURINE SHUTDOWNS' In this section a brief analysis will be made of the expected behavior of the Xe!33 poisoning of the ART during shutdowns. For this purpose the equations derived in Sec. 4 for cases |l and {1l will be employed. First to be considered is a shutdown of nuclear power during which fuel flow and sparging are continued. The reactor is assumed to have been at steady state prior to shutdown. The data given in Table 2 for the ART are chosen, with 7 taken as 5 min. The result is not shown since values for all the terms other than the one for 135 decay are always negligible. Under the assumed conditions, the poisoning will not rise by as much as 1 or 2% of the steady-state valve. It is thus concluded that decreases in reactor power will cause no troublesome transient increase in the Xe!33 poisoning in reactors of the ART type. A more serious problem is concerned with the growth of xenon during a total shutdown. The behavior of the ART is examined in this regard by assuming that after the reactor reaches steady- state operation it is shut down totally and the xenon is allowed to grow in until it reaches its maximum concentration. At this point, sparging is started and continued, at zero nuclear power. It is necessary to determine how rapidly the poisoning can be reduced to the high-power steady- state level. The behavior in this respect governs in large part the amount of ‘“xenon override’’ which must be built into the reactor. The data used are from Table 2, with '7;,=5 min. The maximum poisoning was calculated from Eq. 4.15, After the reactor is shut down, the Xe'3% poisoning rises to a maximum of about 12%. If no sparging were used, it would then decrease slowly, reaching the full-power steady-state value in about 70 hr. During almost all this time, operation of the reactor would be impossible with the control rod presently proposed for the ART. However, if sparging is started at the time of 135 concentration (11.2 hr after shutdown), rapid reduction in poisoning occurs. maximum Xe Figure 13 shows that Xe'33 is reduced to the full-power steady-state value in about 36 min. Since this time is less than that necessary to start up the ART after a total shutdown, '® there seems to be no reason to provide large amounts of ‘xenon override’ in the control rod. This statemen? remains true even if T is significantly larger than the value used here. 9. NOMOGRAMS FOR XENON-POISONING CAL CUL ATIONS Two simple nomograms have been constructed to speed rough calculations of Xe!33 poisoning. Nomogram 1 (Fig. 14) describes the steady-state poisoning (ao + cr.]))\L X & me—— (9.1) )\L+a4+)tp 14 o . . . . . . . . . Although it is somewhat illogical to use the term *‘poisoning’’ in discussing conditions during a reactor shutdown, it is convenient to do so. Difficulties are thus avoided in comparing shutdown con- ditions with those during nuclear power operation, 1 . . 5W. B. Cottrell, personal communication. SSD-C-1209 ORNL-LR-DWG-7316 T '4"tN(]:RELSEI 0|-'I POIISOJ\IIN(l MIAXILAU,\!,, P!OIS(!)NII\!IG @) — L DURING TOTAL SHUTDOWN (ZERO POWER; NO SPARGING)A 1 {2 —= i L~ e — // ¥ 10 , ;’ /] 2 i Z 8 @ £ / o ° 7 M y ¥ 4 / CHANGE OF POISONING DURING SPARGING AT ZERO POWER, SEE EXPANDED PLOT IN (£)~.] A Ly STEADY-STATE POISONING | | /T4~ AT FULL POWER L= It b b L] 0 2 4 6 8 10 12 14 16 18 TIME (hr) 12 (&) 1+ 10 \\ 8 \ g \ () 2 = 3 5 REMOVAL OF Xe'>® DURING ZERO-POWER S SPARGING AFTER A TOTAL SHUTDOWN. T, = 5 min 8 T x \ 4 \\ > \\ STEADY -STATE POlS(m AT FULL POWER ———_ O J l I \\---:‘::-:hfl" 0 5 10 15 20 25 20 15 Fig. 13. Behavior of X During Shutdowns. TIME (min) e 135 Poisoning in the ART 19 #‘3' UNCLASSIFIED SSD-A-1157 ORNL -LR-DWG-6011 O'Xe4> -Dk/k ¢ (sec’) (%) (n-cm 2 sec™) O-Xe — (cm?) (barns) — o7 10° - 2 (499 Y ;'."10 limit ) —10'° (sec™) — Q. — 4.9 —10° \\ = 4 /® —10 1018 106\ - e — Q ; 1014 = \ :—_ //162 ; -2 & l 0'° 10° N 4 — =10~ 10 3 = — 10 - _ \166 = = =— | -20 4 — 10 10 — - — 108 \ 12 — 10 A B 01 6'2 D 20 Fig. 14. Nomogram 1: Steady-State Xe 37 Poisoning. where all symbols are defined in Table 1 and values are given in Table 2. To derive the nomo- gram, let @y + a, U= log |21 _ | (9.2) xw V = log (,\p + a.4) , (9.25) W = log AL . (9.2¢) Then, introducing Egs. 9.2 into Eq. 9.1, the equation for bars B, C,., D of the nomogram is Uu=v-w, (9.3) Furthermore, by letting Z = logoy, , (9.42) S = logd , (9.4b) the equation of bars A, B, C, may be written W=24+5. (9.5) The five bars are laid off with linear scales in the variables S, Z, U, V, and W. The distances between bars is AB = BC = CD . (9.6) To use nomogram 1, lay a straightedge from the value of Oy, ©n bar A to the value of ¢ on bar C,, locating their product (A, ) on bar B. Lay the straightedge from this point on bar B to the value of )Lp on bar D, locating x, on bar C,. The procedure is illustrated by an example shown on the nomogram by faint dashed lines. Nomogram 2 (Fig. 15} describes the approach of the poisoning to its steady-state value. The equation employed is b - E= o memat LD (TR ey (9.7) xoo a - a3 where a =0, + A, + )Lp , % b = — = 0.949 ., D + % To derive the nomogram, let U= e~% , (98a) vo=e 3 (9.8b) ab Wes— (9.8¢) a — 9% 21 UNCLASSIFIED SSD-C-1158 ORNL-LR-DWG-6012 \ A / at t ! a (hr) O'Xed) +)\p (sec) O > —_ O O Q g &4 o | N o I[I|||I|III| IIII| o on O IllJIIlLlilJIJI'IIl_lIllllJ . |'|'|'||||||||||J/'“']""| '|[|'|’|'|'| N O LD Til | | o o \ A o O\ QO ] \ l ~_ CLyv L Q\ ] \ \ ll\lllll_LIm \ i ”llllllll_lj“’l T I'I'I'I'I'I'l o | gun Jlllll/lflill - "lllnll/lullllluu I o N T O — o w *P”L%mlll]l L] o Fig. 15. Nomogram 2: Time Dependence of Xe 37 Poisoning. E=1-U-WU-V). (9.9) Then Eq. 9.7 becomes Further, let Z=WU-V)=1-U~ ¢, (9.10) Bars C,, E,, D, are linear scales in the variables U, V, and (U - V), respectively, the sub- traction being performed on this subnomogram. Since the numerical value of (U ~ V) is not required, no scale is inscribed on bar D,. Bars A, F, D, constitute a nomogram for the operation ] Z o —= (U ~V). (9.11) W Bar A is a linear scale in Z. Bar F is a scale in (1/W), constructed to obey Eq. 9.11, with the Z and (U - V) scales both linear. Bars A, C,, and B constitute a nomogram for the operation Eel-v-1z. 9.12) Bar B is linear in the variable £. The bars C,, D,, E, are used as a subsidiary nomogram to perform the operation log {at) = loga + logt . (9.13) These bars are linear in the variables log ¢, log at, and log a, respectively. The distances between the five vertical bars are AB = BC = CD = DE . (9.14) Bar F is laid off between the origins of bar A (Z = 0) and bar D, (v - V) = 0]. To use nomogram 2, proceed as follows: From bar B of nomogram 1, read the value of L edge from the desired time on bar C, to the value on bar E,, locating the value (at) on bar D.. A, =0y, ® and add to it the value A_. Enter this result on both bars E, and F. Lay a straight- ° P 2 Transfer this value to bar C,. Now lay the straightedge from bar C, to the desired time on bar E,, locating a point on bar D,. Lay the straightedge from this point on bar D, to the value marked on bar F, locating a point on bar A, Finally, lay the straightedge from bar A to the point marked on bar C,, locating the desired value £ on bar B. The procedure is illustrated by an example shown on the nomogram by faint dashed lines. The accuracy of these nomograms is limited by the precision of the input data, the process of drawing, and the means of reproduction. It is believed that the versions given in this report are accurate to around +5%. 23