ML19212A529
| ML19212A529 | |
| Person / Time | |
|---|---|
| Issue date: | 03/14/1977 |
| From: | Levine S NRC OFFICE OF NUCLEAR REGULATORY RESEARCH (RES) |
| To: | Minogue R, Rusche B Office of Nuclear Reactor Regulation, NRC OFFICE OF STANDARDS DEVELOPMENT |
| References | |
| RIL-009, RIL-9, NUDOCS 7912140471 | |
| Download: ML19212A529 (17) | |
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B. C. Fusche, Pirector Office of Nuclear Peactor Regulation R. B. Minogue, Director f
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i FFDP-S. Levine, Director Office of f.'uclear reculatory Pesearch SUFJECT-RESErRCP It:F0 PEAT 0f: LETTEP-9. HIGH TEF*PERATURE 1
CyIIATION f.F ZIPCALOY FUEL CLADDING IN STEAM g
This rrrorardur transmits tha results of corpleted researcF on the hich tenperature oxidation of Zircaloy fuel cladding in stear. This rosearch is aDplicable to ECCS perfomance calculations for light water reactors fueled witt l'-23f>.
The tachnical surrary given in Frclosure 1 presents the major findiros of the work completed to date. The enclosed reports (Enclescres 2-P) are the pertinent cuarterly procress and topical reports outlishad durino the conduct of the research. A final report or tFa isether al and transient oxidation data is scheduled to he published in March, 1977.
The principal results are the follovinc-1.
The rcw date on the isot'erral oxidation rate.of 71rcaloy cladding ir stear. shev a rato cerstant at 22M*F that is only 58 of that of
/
the Eater-Just ecuation, producine-7F of the oxidition that is calculatad with the Cater-Just ecoation. Centacinants in the stearr such as hydronen. nitrocen. and oxygen (from air intrudino durinc a l
LOCA) were found to have no sicnificant effects on the oxidaton behavior.
'Jo observatic effects of stear flow rates were found over the range fror 1 to CG ft/ soc. Particular atterticn was paid to the l
problen of precisr trasurenects of oxidatien rates and raaction ter-peratures. Date r.casurer. ants were r.ada for total oxyrer censured, and for crowth of the oxide and oxycen stabilized alpha phase layers fort ed on tha surface durine the oxidatier. Statistical error analyses were rada of tFe rate deta. and absolute error analyses rade on the terperature rcesurer' ants croducine the Fest charactorized. reliable.
and accurate oxidation rate data yet deterriner' on 71rcaley in steam.
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ur i ce r. Ion tm,*r o er't.s were concucteo in stear usine transient tirc-tamarature histories for postulated LrCA's. The exparirentally daterrinad isntharval oxir'itien rata date were then used in a corruter codo to calculete the oxidation excacte'd durine the experirental transient tests.
'"b e. experirant?1 results acroac' with thosa predictad by the code, thes varifyf ro tSe usa of the isotFarv el rate data in calculetira the arourt of cyidatice duriric postulated reactor accident':.
3.
- n autn-catalytic roection of the srecirers vas net et sarved in any experiront, thourh uncridized srarfrars were heata in flcwinc stear frer about annar to as hich as 27 9'r in as little es ter sacer.ds.
and ir a feu cerns were plurced ir a fraction of a spennd f eto flowinc stear 1r a furnace hr 1? at 200r*F. Sore spacirer, Snatinc above the desired raactinc te:porature was of servad, but each speciran cuiclly cocled to the reactior tV nerature and icnition did not occur.
t.
Tha rate of diffutien of oyverr in 71rcelov at hinh tenneratores (beta phasa) was fann? te he arnroxirately oneIbelf that previously reported in the literat"re an<' usad at this tit c in Fest estirato a nc' avsluatier rodel calculeriens of erbrit+1crent of fu-1 eleddine durire a postulated !Or.'.
narticular attontion was paid to the orchlens of reasurecents of diffusion rates and tarpereturas. Threr iridenerdant ret %ds of deter-tre. tion vare usad in the diffusivitv stu?y. W cxcalient arrearant of the data fror tbr thrne ine'enardant rotbeds.
es shown in %fere ca f,19('icatas that tha ner data arr free frer systematic errors.
fvaluation and ornficabilftv 4
1.
This crocrar and its results havn been ravie.t ed ranastedly whila in crorress by the 71rcalny fladdinc r.pyjer e rnu. at cuartarly 7ircalny Claddine rrocrar "evice rantinos and at tFe 4crunl Pater raector Safety Pasea rch Inforration *~eetine s.
'nterastad verders. nu'lic, and sciratists fror other orraai7ations hava atter.ded both. 7a quarterly and topical reports issuad hava received UPC-3 distributine (32" cepfes) trd hava been obtained froo *!TI" by nurarn'rs researchers in both this and other countries. Tha consensus has been that t!.c work has beer conducte<'
corretently and with sufficient ettention to technical detail. nrecisier, and accuracy. Extrane care was talrr to elirinato the uncertainties in terceraturr rresure ent charactoristic of the data previously reported..The nrv oxidaticn rate data havn haen confir ed by r nrc limited stwfies in.? aran and ren:ary.
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The iroact of tha new data on LOCf analyses was exarined bv cal-culatinc peaf claddire termeretures usinc both the new data and the Frier Just correlation ir. a FPf.P-T3:RElaF a corruter code sfrulation of er experinertal lnC' tost conducted srvaral years aco. It calculated claddiec terparatures neer 2200'F, tFe naw eovatfor predicts a tercera-tura l!'F 1r+.'ar ther that credicted usine the raker-Just correlation. -
3.
The reduras rata o' heat ceraration as calculated usine the new data, alone with the experierntal chservations. irdicate only a srall prot. ability of rossible icnition of the fuel claddine durinc a LOCA. ~
Ir additier, tha erreriNnts indicate that the cxide filr forrod on the fuel rods hy corrosien durinn norral craration should cause a sierificant dacressa ir tFe total oridatfrn occurring durine a nostulated accidant fror that calculated usine unexidi7ad foal claddirc.
4.
It was obsarved that an additieral conservatisr ray soretires occur ir tbc annlication of tha isothe..al rate data to LOCf calculations.
In instancas where (a) the first ter ocrature peat in the LOCA is craatar thar a!'ont 1MP'F (F) the followine tornerature r"inirrir is 1 css that a'ou* lW'r. and (c) tbc sacond tornerature peek is less then about 77oa'F, t&c exrorir antally obsarved consurstion of oxvnen is sianificantly less than that calculated usine the isothen al rate data. as is th9 thictonss of tFe orido filr. Povever, the tFiciness of the oxyran stabilized alcha layer enrears to be increase? alrost ds ruch as the thicinoss of the oXido layer is drCreased. so that t"9 thickrass of ductilo wall laft to sustain loads is alrost unchanced.
It is tFoucht that tN' '~anoralous cridatten effact is duo to a recently discovaroM hysterests ir the-phase transferntions of tre nxida file at f
tevaaraturvs t etwanr aSur IF~ and P2nc'F.
r,. The present TCCS f,r.c'ntanen Criterie place tbe licitaticas of 22Pr*F peat cleddirr treocrature and 17r equivalent oxidation of t% eall tr. iciness to lirit tha decree of er brittlerent of the fuel claddino durinc and after a 10CA. Evalcation rodels frequently use the prasant literature dato on the diffusivity of crycan in heta phase 71rcaloy.
in addition to tN thicinasses of oxide ed oxycon stakilized alpha phase calculatad. to estimato the depth of oxycen cenetration into the beta phase fror tha alr.ha-beta interfaca. Thay than estireto tFe wall thief ness of ductile wall rerainino to sustain loads fi resed durin" and after refloodinc of the coro. The raw diffusivity data indicate that there wculd be sicnificantiv less depth of arbrittler ort in the fuel claddinc wall calculated for an civo
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e cor$1ned with the rato data determined on the growth of oxide and oxygen stabilized alpha layers, will produce a more scientific base for establishiro erbrittlenent criteria for ECCS Accectance Criteria.
These results have been obtained in response to the specific directive civen PTS by the corr.issioners to obtain new, better, and better-characterized data on the oxidation rate of 71rcaloy in stear. They confirr that thera is a larce deoree of conservatisr in the evaluation j
model beinn u' sed by the Pegulatory Staff for calculatine the oxidation of Zircaloy durino a LOC.a. RCS will be harry to furnish you any cooperation and assistance that you may recuire in plannine for a l
chance ir the ECCS acceptance criteria in 10 CFP 50 f reendiy V.
Original Signed by Saul Levine Saul Levine,.nirector Office of Muclear Pequiatory Pesearch See naxt pace.
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DISTRIBUTION:
B. Burson, RES SUBJ R. Foulds, RSR CIRC C. Beck, RES CHRON G. Bennett, RSR MLP rf 7!
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Enclosures:
1.'
Appendix 1-Tecbrien1 Surriary - Hich l a'Vera tura x1 cat 1cn of 41 rca loy Fen 1 Claddinq fr Staer
?.
J. ". Cathcart, "funrterly Procrass t'arcrt nn tha 71rconf or t'etal-
"ntar f xidetion Vinetics Pror'rar-Sponscred by the ' et Division of Peactor,afo'v rescarch for e
January-Parch in7r, on','t /.' t'Rir/
TF-17, t'av 197f 3.
J. V. CetFeart, nuartarly Procross PeDort on tha 7t rconitra "ctal-Water rxidatice Pinctics Prorra' Focnsorad Fv tha "PC *iivision of Feacter Fafety rasnerch for
- n ri l -.ic n a in7f, AR"I./i.'t'P.Fr/
TP al, Junust in?F 4
J. V. C*theert #uarterly Ircorass Report on the 71rconim "etal-
'!ater '.xidation "inatics Procra Sponsora? by t"a M Divisior. of Opactor Rafarv rataarcF for July-Senter her 197f. ';P' ! /' t'pr/
Te.rp, ecert9r 1r76 h.
J. V. Cathcart, et. al.. Zirenrier f'etal "ater 5xthtien Einetics I.
Thnmo ntry.
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ic5ruary lo7f f.
F. '. Pattirs. Zirconiur "etal-7 Petar fridation Einetics II.
0xycan-1P "irfesinn in Rota Zi rcelov OP'1/'.'UPEC/Tf'-19, iluly 1976 7.
- r. T. T wel. 71 rceniur "e tal-
a tor 9xidaticn Rineticr. III.
r ido and 1568 107 Axycan riffusion in x
t1pf.a 71rcalev rhaus, OR'.'!./
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S. f'alenn. SI'1r I - A Cc o star redo for tha Struitaneous Cr1-
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JU and Tercperature Profilas in m
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Addressees
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MAR 14 1977 l
cc w/Fnclosure 1:
V. Stello, 00F R. Heinerran, DSS D. Ross. CSS F. Coffir.an, 00R R. Meyer, CSS G. A. Arlotto, SP i
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ENCLOSURE TECHNICAL.
SUMMARY
HIGH TEMPERATURE OXIDATION OF ZIRCALOY FUEL CLADDING IN STEAM This sumary transmits part of the new information obtained in an RES-sponsored research program on the rate of oxidation of Zircaloy fuel cladding in steam and the rate of diffusion of oxygen in beta phase Zircaloy. We believe the new data should allow quantification of the conservatism of the required use of the Baker-Just rate constant equation for calculation of the rates of oxidation of Zircaloy, as stated (Ref.1) in the present ECCS Acceptance Criteria.
In Docket No. RM-50-1, Acceptance Criteria for ECCS in LWP, the Con-missioners of the AEC stated (Pef. 2):
"This ecuation was derived by Baker and Just from their measurement of the rate of oxidation at the melting point of zirconium, in conjunction with Lemmon's and Bostrom's data at lower temperatures. The eouation is a straight line representation of a plot of the logarithm of the reaction rate vs. the reciprocal of the absolute tempera-ture. The slope of this line is the activation energy, and depends in an imoortant way on the single point of Baker and Just at the melting point of zirconium."
~'
"The Baker-Just equation has been criticized extensively,...
"Until new data are obtained and present doubts are resolved we believe it b~est to continue the use of the Baker-Just equati on. "
"There is evident need for new and better experimental data to resolve this issue and to provide a rate equation with a more representative activation energy...."
1568 109
h I They also directed (Ref. 3) "...the Director of the Division of Reactor 3a.~ev Reseor ui w yive priority attention to study to determine more exactly the temperature at which clad embrittlement ceases to be siraply a function of oxidation". A confirmatory research program sponsored by RES and nearing completion at ORNL has provided new data and rate ecuations pertinent to these needs.
The principal results are as follows:
1.
The rate constant
, 6:, for total oxygen consumed during the isothermal oxidation of Zircaloy-a in steam at atmospheric pressure has the temperature dependence from 1832'F to 2732*F (Ref. 4,5) 2 22 gr /2 = 0.1811 exp [-39,940/RT)
(g/cm ) /s.
For comparison, the Baker-Just equation (Ref. 6) in the same units is 2
22 6 /2 = 2.0496 exp [-45,500/RT]
(g/cm ) /s.
7 Eotations of the same 'orm have been developed (Ref. 4,5) for the thicknesses of the(g gen-stabilized alpha layer, the oxide layer and the Xi layer The new data are reported graphi-cally in Figure 1.
2.
The diffusivity of oxygen in beta phase Zircaloy-4 was found (Ref. 7) to have the temperature dependence from 1832*F to 2732*F 7
-2 2
D = 2.63 x 10 exp [-28,200/RT]
cm /s for oxygen-16.
The values of the diffusivity of oxygen in this temperature range are approximately one-half those reported previously for Zircaloy-2 by Mallett, et. al. (Ref. 8). and now used for calculating the oxygen gradients in the beta phase of oxidizing cladding. The data are compared in Figure 2.
(a) for the parabolic rate ecuation W = 6 (T, with W = grams of oxygen censumed, t = seconds, and 5 = the parabolic rate constant.
(b) the Xi layer thickness is the sum of the oxide and alpha layer thickness.
1568 110
> 3.
Two comnuter endas. STMTRAN T (Raf. 4) and RTI D-R (Raf. 10) ha"a been written for calculating total oxygen consumed, alpha and oxide layer thicknesses, and the distribution of oxygen in the beta phase during postulated temperature transients. SIKTRAN-I will also calculate temperature distributions in the fuel cladding during the temperature trar.sients, but it reautres more time to run.
Both codes have been verified with experi-mental data obtained in transient temperature oxidation experi-ments at ORNL.
The new oxidation rate data are compared in Figure 3 with the J2ker-Just (B-J) rate equation and with data recently reported by other investigators.
At 2200*F, the new data show a rate constant for oxidation 58% of that calculated by the B-J equation. The new ORNL data have been essentially r
confirmed by data recently reported by Kawasaki (Ref.11,12) and by Leistikow (Ref.13) and the disagreement with the B-J correlation con-firmed by data reported by Heidrick (Ref.14) and by Biederman (WPI) et. al. (Ref.15). The new data also agree quite well (Figure 4) with the oxidation data reported by Hobson and Rittenhouse (Ref.16) as recalculated by Pawel and Hobson (Ref.17).
Extreme care was taken in all experiments to be certain of the accuracies of the temperature measurements and to allow the conduct of statistical evaluations of the experimental data.
The absolute errors in tempera-ture measurements were within +7.2*F pt)for the rate constant 6 /2 1652*F and within +10.8 F at 2732*F. The 90% confidence intervalssc 2
s cal.ulated by the new rate equation are +3.3% at 1922*F, +1.7% at 2192*F and +2.9% at 2732*F. Admission oT 5% hydrogen,10? nitrogen, or 10% oxyge,n te the flowing steam had no definitely measurable f
effect on the oxidation rates. Steam flow velocities from about 1 ft/sec to about 90 ft/see had no observable effect.
An experimental simulated LOCA test, FRF-2 (Ref.18), has been modeled using FRAP-T3 and RELAP-4.
Calculations were made of peak cladding temperatures and total oxygen consumed using the B-J correlation and then repeated with the new Cathcart-Pawel (C-P) correlation substituted for the B-J equation (Ref.19).
These values were then used to estimate the thicknesses of the oxide and oxygen-stabilized (c) The physical significance of the 90% confidence interval is that if the experimental data were redetermined under the same conditions by the same techniques as that reported, there is a 90% probability that the best estimate line for the new data would lie inside the intervals specified.
1568 111
. alpha layers, the Xi tnickness, and the, thickness of beta phase remaining, assuming an original wall thickness of 0.025 inches. The resu'lts are given in Table I.
At 200 seconds into the calculated LOCA, the peak cladding temperature was 2335 F using the B-J correlation and 2232*F using the C-P equation. The reduction in calculated peak cladding temperature using the new date in this model was approximately 100*F. The wall thicknesses consumed were 10.3%
and 6.5%, respectively. While the oxygen profiles in the remaining beta phases were not calculated, the new diffusion data (Ref. 7) show that the depth of contamination would be considerably less (the diffusion rate is approximately one-half that previously reported by Mallett (Ref. 8)).
In the determination of the new diffusion rate data, the absolute temperature errors were within 1.1.8*F at 1652*F and 1.3.6*F at 2732*F.
The 90% confidence intervals for the diffusivity, D, of oxygen in beta phase Zircaloy-4 are +7.8%, -7.2% at 1832*F, +4.2%, -3.9% at 2282*F, cnd +10.0%, -3.1% at 2732*F. The new data were obtained by both tracer and chemical diffusion data (no statistically significant differences) and the diffusivity was found to be independent of oxygen content in the beta phase.
A final report on these parts of the ORNL study will be issued by March 1977.
I f
i568 112
J
. s REFERENCES 1.
10 CFR 50 Appendix K, Section A.S.
Metal-Water Reaction Rate.
2.
Docket No. RM-50-1, 28 December,1973 "Acceotance Criteria for Emergency Core Cooling Systems for Light-Water-Cooled - Nuclear Reactors: Opinion of the Commission", Paul C. Bender, Secretary of the Commission, III. A.5.
Discussion: Metal-Water Reaction Rate, pages 56, 57. 58.
3.
Ibid., I.
Introduction, p.10.
4 ORNL/NUREG/TM-41, " Quarterly Progress Report on the Zirconium Metal-Water Oxidation Kinetics program sponsored by the NRC Division of Reactor Safety Research for April-June 1976", August 1976, J. V. Cathcart.
5.
"Sumary of the Zirconium Metal-Water Oxidation Kinetics Program" J. V. Cathcart, et. al., Fourth Water Reactor Safety Research Information Meeting, September 27-30, 1976, National Bureau of Standards, Gaithersburg, Maryland.
6.
ANL-6548, " Studies of Metal-Water Reaction at High Temperature, Part III: Experimental and Theoretical Studies of the Zirconium-Water Reaction" May 1962, L. Baker, Jr. and L. C. Just.
7.
ORNL/NUREG/TM-19, "7irconium Metal-Water Oxidation Kinetics Part II: 0xygen-18 Diffusion in Beta-Zircaloy",, July 1976, R. A. Perkins.
8.
J. Electrochem Soc. 101:
181-84 (1959) "The Diffusion of Oxygen in Alpha and Beta Zircaloy-2 and Zircaloy-3 at High Temperatures",
7 M. W. Mallett, P. Albrecht, and P. R. Wilson.
9.
ORNL-5083, "SIMTRAN I - A Computer Code for the Simultaneous Cal-culation of Oxygen Distributions and Temperature Profiles in Zircaloy During Excosure to High-Temperature Oxidizing Environments
November 1975, S. Malang.
- 10. R. E. Pawel, ORNL, unnublished,
- 11. JAERI-M-6181, " Reaction of Zircaloy Cladding with Stean Under Simulated Loss-of-Coolant Accident Conditions" Saturu Kawasaki, Teruo Furuta and Masao Hashinoto, July 1975.
1568 113
t q '~. 12. JAERI-6601 "Zircaloy-Steam Reaction and Embrittlement of 0xidized Zircaloy Cladding in a Simulated Loss-of-Coolant Accident" T : ;,.";c t:, 0:.tu. ; lO..s;.:d,.*t;.e ll:.s. *... :.
..J To' o.:. ; 0 ;.v..,v,
June 1976.
- 13. Leistikow, S., GfK, Karlsruhe, FRG, personal comunication to J. V. Cathcart, ORNL.
- 14. Heidrick, T. and Urbanic, V., unpublished AECL data.
- 15. Biederman, R. R. Third Interim Progress Report, July 1 - September 30, 1975, "A Study of Zircaloy-Steam 0xidation Reaction Kinetics,"
EPRI Project 249-1, Worcester Polytechnic Institute
- 16. ORNL-4758, " Embrittlement of Zircaloy Clad Fuel Rods by Steam Durina LOCA Transients", January 1972, D. O. Hobson and P. L. Rittenhouse.
17.
Unpublished, R. E. Pawel and D. O. Hobson, ORNL, 1973, oxidation data recalculated from data originally reported in ORNL-4758 (Ref.16).
- 18. Nuclear Technology, Vol. 11, No. 4 (Aug. 1971) pp. 502-520,
" Fuel Rod Failure Under loss-of-Coolant conditions in TREAT",
R. A. Lorenz, D. O. Hobson, and G. W. Parker.
19.
Private communication, L. J. Siefkin, INEL (EG&G) to M. L.
Picklesirer, NRC, December 16, 1976.
7 1568 114
Table !
Cal:ulation(a) of Damage to Cladding During Simulated LOCA Using New and Old 0xidation Correlations Time into LOCA, lec 25 sec 50 sec 100 sec 150 sec 200 sec Correlation Equation (b) 8-J C-P B-J C-P B-J C-P 8-J C-P B-J Ch Peak Cladding Tenperature F 1603 1603 2247 2217 2296 2247 2323 2247 2335 12
~
Thickness of wall consumed, mils 0
0 0.633 0.457 1.50 1.02 2.08 1.38 2.57 1.64 Thickness of wall consumed, %(c) 10.3%
6.55%
Equivalent oxyge1 consumed.
mg 0 /cm2 13.9 8.9 2
Estimated oxide layer thickness, mils 2.75 1.72 Estimated alpha layer thickness, mils 2.99 1.87 Estimated Xi layar thickness, 3.Sh mils 5.74 Estimated Xi layer thickness, %
wall (c) 22.9 14.4 w
Estimated thickness of beta CD Zircaloy remaining, mils 19.3 21.4 W
(a) Using RELAF-4 and FRAP-T3 modeling of FRF-2 (see Ref.18)
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(b) B-J = Baker-Just correlation C-P = Cathcart-Pawel correlation (new data)
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(c) assuming wall thickness of 0.025 inches
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Figure 2.
Diffusivity of Oxygen in Beta Phase Zircaloy-4.
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COMPARISON OF DATA u
TOTAL OXYGEN 5
RATE CONSTANT O
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Figure 3.
Arrhenius Plot of 0 idation Rate Data for Isothemal 0xidation of Zircalcy-4 in Steam, Total Oxygen Consumed.
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'/r (*K 'X 10 )
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Figure 4.
Arrhenius Plot of Isothermal Rate of 0xidation of Zircaloy-4 in Steam, Comparison of Equations.
9 1568 119 g
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1568 120
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