ML19323B868

Forwards Draft Results of TMI Bubble Analysis Investigation. Estimates That 450 Kg Hydrogen Was Produced by Oxidation of Zircaloy Fuel Cladding.Repts on Computer Simulation,Hydrogen Bubble & Hydrogen Burns Encl

ML19323B868
Person / Time
Site:	Crane
Issue date:	10/15/1979
From:	Cole R SANDIA NATIONAL LABORATORIES
To:	Picklesimer M NRC - NRC THREE MILE ISLAND TASK FORCE
References
TASK-TF, TASK-TMR NUDOCS 8005140366
Download: ML19323B868 (20)

Text

.

/

Sandia Laboratories Albuquerque, New Mexico 87115 8 0 0514 0 3Zo(p October 15, 1979 Dr. M.

Picklesimer NRC/TMI/SIG Rm. 412 6935 Arlington Road Bethesda, MD 20014

Dear Dr. Picklesimer:

Enclosed are the results of our TMI Bubble Analysis investigation.

The stated objectives of the' project were:

1.

Determine the quantities of non-condensible gases formed and how they were formed.

2.

Determine the time distribution of non-condensible gases in the primary system.

3.

Determine distribution of gas between reactor primary system and containment.

Our conclusions, as previously reported by telephone, follow.

Several aspects are expanded on in the attachments.

Our best estimate (based on previous work and a new computer calculation) is that approximately 450 kg of hydrogen was produced, essentially all by oxidation of zircoloy fuel cladding.

A small amount (less than 10 kg based on rates

" Core-Meltdown Experimental Review" SAND 74-0382, August 1975) could have been produced by oxidation of stainless steel.

We concur in the general conclusion that radiolysis was not important and that there was never any significant amount of free oxygen in the primary system.

Of the total hydrogen, we find that approximately 300 kg was released to containment before 9 hrs., with the remaining approximately 150 kg removed over the next several days.

These results, from the computer simulation, are reasonably well supported by a back calculation from the hydrogen burn at 9.9 hrs., and by extrapolation of bubble sizes measured later.

Dr. Picklesimer The chemical results are inconclusive.

Radionuclide con-centrations in the primary system are consistent with the calculated core damage, if it is assumed that a significant fraction of the 270,000 gal of water from the BWST somehow did not pass through the core.

It appears that leaching is as likely a method as volatilization for removal of some of the fission products from the fuel, so.that one need not infer extended periods of extremely high temperature.

We were unable to find any satisfactory explanation of measured boron concentrations.

Some of this work, in particular, the computer simulation and the bubble calculation, will be expanded during the next several weeks.

New results will be reported as they become available.

Sincerely, Randall K.

Cole, Jr.

Reactor Safety Studies Division 4441

Enclosure:

1)

Computer Simulation 2)

The Hydrogen Bubble 3)

Hydrogen Burns

R.K. Cola, Jr.

SCndin Lths, Albuqucrqua.N.M.

14 Octobar 1979 COMPUTER SIMULATION A computer code was developed, prinarily by Michael I Baskes of Sandia's Livernore Lab, to provide a simplified model of the TMI2 reactor coolant system.

The code uses all available data including pressure, tenperatures, pump flows, and valve positions as input.

It calculates core response and hydrogen production, and water and hydrogen inventories in various compone fts including the reactor vessel, hot and cold legs, steam generators, and the pressurizer.

Both mass and energy conservation are considered for the reactor vessel.

Core physics was initially treated much as described in NUREG/CR-0913*, including finite heat transfer coefficients between fuel and liquid and between fuel and steam, but neglecting the radial power profile.

For all 9\\

other components, mass alone is conserved.

Flow through f

s the PORV is evaluated using HEM critical flow and an effective

(

k (O

area of 1.09 in2**.

'y j

Calculations with the original core model predicted V bk s

hydrogen generation shortly af ter 2 hrs at such a rate that

%4 C h]V

'R the calculated partial pressure of hydrogen exceeded the 00 l

q, h

measured cotal pressure.

The model was therefore modified 1 g, NS 4

W

\\

to consider the flow of molten zirconium clad down the rods to cooler regions of the core, delaying its oxidation sufficiently to eliminate the contradiction.

The relatuive ease with which

• R.K. Cole,Jr., " Generation of Hydrogen during the Firnt Three Hours of the Three Mile Island Accident",NUREG/CR-0913, SA'm79-1357, Sandia Laboratories, Albuquerque, NM, July 1979.

• • Reasonable results could not be obtained using the 0.87 in2 ef fective area of NUREG/CR-0913.

R O U G H D 3 A F'..

ROUG3 D: RAFT

-t-this modification could be made results from the basic structure of the code.

The various relationships to be modelled are represented by a set i of ordinary differential equations (the current version employs more than 100) and solved by a general purpose library routine.

This routine and controls the time step by monitoring its own accuracy, will terminate (with appropriate messages) if severedifficulties are encountered.

hours of the accident Pp'eliminary results for the first 6

/

are shown in Figs 1-3.

We anticipate that during the depressurization between about 7 and 9 hours1.041667e-4 days <br />0.0025 hours <br />1.488095e-5 weeks <br />3.4245e-6 months <br /> approximately one half of the hydrogen remaining in the reactor vessel and steam generator B will be inst, leaving about 150 kg in the These figures primary system and about 3JO kg in containment.

are consistent with back calculations based on later bubble sizes and on the hydrogen burn just before 10 hours1.157407e-4 days <br />0.00278 hours <br />1.653439e-5 weeks <br />3.805e-6 months <br />.

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$b Albuquergua N.M.

UJ 12 October 1979 THE HYDROGEN BUBBLE During the period fcom 29 $ arch through at least 8 April measurements were made to determine the size of the (ass umed) hydrogen bubble in the TMI2 reactor coolant system (RCS).

The procedure was to define a mass balance for the RCS (exclusive of pressurizer) by recording changes in the levels of the pressu pressurizer (PZR) and makeup tank (MUT).

From this, the change i

in bubble size (and therefore the apparent compressibility) could be calculated and the bubble size inferred.

We have independently 63 rived a " bubble formula", compared it with the Met Ed and B&W formulae, and used it to reduce the

)

raw data in the " Bubble Book".

The total hydrogen content of the RCS, including hydrogen in solution, was then fit as by a rex straight line (as a function of time) to estimate the average removal rate.

THE BUBBLE FORMULA We assume that the bubble is a mixture of hydrogen gas and water vapor.

Because of the low temperature and water vapor pressure (280 F, 50 psia) Dalton's Law should apply.

The zh change in water vaporTdue to the partial pressure of hydrogen

• ssare

{- ?g (T) x (P-% CT0 Q{ Q Q) is negligibly small--about 2 psi at a total pressure of 1000 psia.

The partial density of water vapor in the bubble is essentially the saturation density oj vsat (T).

The total water mass in the RCS is given by

• P.M: Morse, Thermal Physics, W A Benjamin Inc, 1969, p124.

ROUGH DRAFT

~

~

~

ltOUGH DRAFT g'. cv <v)pp"'f r '%v"g,,,, cr"'9.

a a

If Eq 2 is evaluated for two (P, T) states and the results subtracted, one finds R es ges RG be ek 6*-(frf<),

V,"=Op-k),go-(V,-fQ

. 6) p Witha the general notation (f is ang gu e n /e*/ )

7 f5 (Ss V YvY2-()

1. R-9, m

Eq 3 becomes g-fg)bY +

b {fff4 Ofg fj.

b

~ON

$)

=

This equation (which contains no approximations) may be h

simplified by elimination of several small terms.*

At 1000 psia 3

3 and 280 F, hts 8lb/ft and g

.12 lb /ft Also, V 210300 ft m

B and (we will find) V is typically several hundred cubic feet while Af is typically a few thousand pounds for a pressure change of 100 psi.

The expansion of a cylindrical vessel is jihen h av#2 F T v pj where R/t is the ratio of # radius to thicknes, about 8 for the RCS, and E is Young's modulus, roughly 3x10 psi for steel.

Thus AV is typically 30 lb, a 1% effect.

Temperatsre changes were almost never greater than 1 F.

Therefore, from Steam Tables,wefindgd.05lb,/ft and $ [.002 lb,/ft Thus 8 A(

is a few tens of pounds, again a 1% effect, while V

A may be several hundred pounds and is significant.

Finally, neglecting compared to we find

• The reader may skip to Eq 8, an obvious approximation, and miss only a discussion of the accuracy of that approximation.

fcS h

[W ROUGH DRAFT pa g

ROM D3 AFT sv % (v "'%pl".- af'.)/7lc>

c,y accurate to a few percent.

The mass increase in the RCS is simply the net mass loss from makeup tank and pressurizer, reduced by net leakage.

Because the pressure and temperature in the makeup tank are essentially constant the change in its density may be neglected, but this is not the case for the pressurizer.

The resulting expression is an,R'% - (p A s-)#- b(Q <-f, Vu) PEA Ae<k Here M

o

\\fft R, {g (g_,g )~1 y PtR., y ER_ \\f, PH-(

P L's are levels, where the A's are horizontal cross-sectional areas,/L is the g

effective height of the hemispherical section of the pressurizer below the lower sensing nozzle (2/3 the radius or 28 in) and Akeak is the unknown leakage term.

The hydrogen content of the bubble is simply M '* Pn V"/RT Iv{QG; u

moles where R is the gas constant and Pu = P-P,a (T)

(13,J is the partial pressure of hydrogen.

The solubility of hydrogen is proportional to its partial pressure and (neglecting the

/

compressibility of the water) is given by (T) P m les per H

unit volume.

The total hydrogen content of the RCS (exclus ive of the pressurizer) is given by g7

+ 4b (T) Pp (V

-V WW n

tny assuming that a bus $le is present.

Ifn)seliminatedfrom 14-L2 Eq 45 by using Eq yr, the resulting equation is v"

l D -J'RT)P. - l'n~ v">o~

($

' 4""

y

)-4 'R T ROUG3 DRAM

_4-ROUGH JRA"W-where the dimensionless quantity

.2'nr=.2 % / % /nr)

G6) is simply the ratio of the volumetric concentration of hydrogen in solution to that in the vapor phase, and is approximately 0.03 at 280 Ft Equation 1[ explicitly includes the possibility that all hydrogen is in solution with no bubble present.

If measurements are made at two pressures but nearly equal e/

A temperatures so that changes in 4 and T may g be neglected

)

Eq lgmay be used to show that**

gfg

-tnas -L Pso,

> Ho in(I6 V

?

+ 5Yb l

I A

ps s

N E

and P is the lesser 0 where the bnotation of Eq 5 has been used/ OnchEhetotal I7 hydrogen content of the system has been calculated from Eq MP, Eq 1[may be used to calculate the size of the bubble at any pressure.

If a bubble is present in both states 1 and 2, the 17 first term in brackets in Eq 96 is the greater, and the bubble volume is given by k 'RT

& JPg Pg P flW y,

Pu %

AV

• l#d 'R'4 "'

B

- pp b 69

\\

If a bubbig is present only at the lower pressure, the second ih Egri term /is the greater, and V

[IJ,, fle a) V,,,,,'n yhp b

• • • " lbY

\\f r

w Finally, if no bubble is present in either state, Eq yields an the upper bound on hydrogen content given by the amount soluble 17 at the lower pressure, and Eq 47t gives zero volume for any pressure about which we have knowledge.

In practice, because of experimental errors, it may be difficult to distinguish the latter

• Calculated from H.A. Pray et al, "$olubility of Hydrogen, Oxygen, Nitrogen, and Helium in Water", Industrial and Engineering Chemistry 4

(5) 1146-1151, 1952.

R4

• • We assume that )QQCIE ft is constant during the measurement.

Changing hydrogen content could be included with minor changes in the following equations.

{

KU ugh. UKk 1

-su RCS two ccaco, cnd it m y be bettor to interpret n En fr m Eq IS 87 H

ss an upper bound whenever the second term dominates.

For the case where a bubble is present at both states 1 and 2 is our aquaki bubble formula / given: Ly Eqs 8, 9, and 19.

The B&W formula is in close agreement, although matching the solubility terms takes a little work.

The main differences are B&W's neglect of changes in vapor mass in the pressurizer, and of liquid below the lower sensing nozzle (L in Eq 10), which are offsetting effects of a few percent each.

Also, they appear to use total their equivalent of pressure rather than hydrogen partial pressure in/Eq 18, which would lead to a 5% underprediction of bubble size.

Surber The Met Ed formula also uses total pressure, and mibee neglects all compressibility and thermal expansion terms for the water.

neglected The most important of these terms /is thermal expansion in the pressurizer under increasing saturation temperature, leading to a 10% underprediction of bubble size.

The next largest term, Res Ah is dominated by temperature changes and therefore not consistent in sign.

Much more important is the :- ;':-

neglect of the solubility of hydrogen.

The effect is shown by the last 3

term of Eq 18 to be a systematic 300 ft overprediction of bubble volume (d RT %.03 and v h10300ft ). While the previously mentioned errors tend taxpradura toward underprediction, they are substantially overpvs 4 M 4,, M eeg 4 FAe smaller so that theMeglect of solubility is the overriding esseer.eQped, i

Finally, the innexxxMMX data reduction in the BuMle Book contains a number of arithmetic and/or transcription errors.

Y bh{

w'<

V 1

C-R. O.UG2 DRAR RESULTS The bubble formula derived in the preceeding section has been used to reduce the raw data presented in the Bubble Book.

The mz RCS temperature and the makeup tank temperature were taken as 280 F and 80 F, respectively, when these data were not recorded.

We observed that the pressurizer temperature and system pressure were not consistent in that the pressure was ~ consistantly 50 psi lower than Psat (TPZR).

This discrepancy, I

in the wrong direction to be explained as by a partial pressure of hydrogen, could be due to a 5 F error in T However, we also noted that for the earliest data sets pressure was reported from the wide range recorder as well as from the computer, and is typically 50 psi higher.

This problem has not been resolved.

Therefore, in those cases where T was reported as well as P, the pressurizer mass term ha was evaluated twice, first using P m,ef to determine saturation densities and then

, and the average used.

In no casa was the difference significant.

The results of these calculations

• are presented in Figures 1-3.

The first shows total mass while the second and third give bubble volumes at the average system pressure of 1000 psia and at the Meted-established standard 875 psia.

Also shown in these figures Tre the generalized least-squares fits to the data from 3/31/79 through 4/3/79 with an approximate one-standard-deviation confidence band on the fit, and a fit presented by B&W.

• The mass-leak term was taken as zero.

We intend to repeat the calculations using the value mentioned later in the text.

l

• • The generalization involves points where the bubble was"alnest gone", and the fromula yields an upper bound.

• • • Memo from James H. Taylor to John Bickel, 20 July 1979.

We consider only the data "With Solubility Correction".

RO3GE drain ROUGH DRAM We feel that the difference between the two fito may be due to

't B&W's apparent use of only 5 data points.

The standard deviation of the points used in our fit from the fit line is i 12 kg, in reasonable agreement with the error bars shown by B&W, corresponding to a mass error of I 8 kg.

We find an average removal rate of 1.7 (*0.3) kg/hr.

This corresponds to the complete degassing of 60 (*10) gpm of letdown flow.

This is not meant to imply that all the hydrogen was removed through letdown, but merely to note that typical letdown rates are sufficient to remove most of it.

For comparison, the B&W line implies i a significantly larger removal rate of 3.0 kg/hr, again perhaps due to the small data set used.

Our fit suggests that the bubble was gone at 1000 psia at 1800 on 4/1/79

(. 3 hrs ).

During this time period the pressure i

was being cycled between about 950 and 1050 psia.

The bubble would be eliminated at the higher pressure about an hour earlier.

If the constant removal rate is used to estimate the hydrogen content of the RCS at 16 hour1.851852e-4 days <br />0.00444 hours <br />2.645503e-5 weeks <br />6.088e-6 months <br />s--a very questionable extrapolation o

naccurate data--one finds a total mass of 190 (*40) kg.

At 0

1400 psia and 360 F a there would be be roughly 45 kg in solution 3

and an 1100 ft bubble.

Two or theee hours later when the pressure had fallen to 1000 psia, and the temperature was also lower, we would estimate a bubble size of 1300 ft3, We have not included the effects of any leakage of water or loss of hydrogen during the course of a measurement.

The former clearly exis ts :

An analysis in the Bubble Book shows R03GH DRAM l

RG3GE DRAr 1

~*-

replenishment of the makeup tank at an average rate equivalent 3

to 46 ft /hr at RCS temperature and pressure.

The excess over 3

N the bubble shrinkage rate of 16ft /hr atx is presumably ana'ccounted

/

leakage, a mass loss of perhaps 1700 lb,/hr (3 or 4 gpm).

This is confirmed in the data reduction in that, for cases where it.

is clear that no bubble exists (on 4/2/79 and 4/3/79), the RC1 still appears to accept an excess 500-1000 lb of water during m

a typical pressure excursion.

When time permits, we intend to repeat the analysis, including this average leakage rate in the mass balance from which the bubble size i inferred.

We do not anticipate any large change in results.

0

(

ROUG3 DRAFT

~'

RO"JG3 DRAM MODIFIE0 AREAS, RHOS, CORRECT PRZR, COMP,PP SOL 1.300 m+

o 1.200 x

1.100 1.000

.9000

(

.8000

\\g

\\

\\ \\\\

.7000

\\

\\

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\\\\\\

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\\

)

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• \\ g*

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',^ - f*

0.000

.1000 "O

.'000 i i

.i i

i 0.00 50.0 100.

150, 200.

250.

300.

HOURS AFTER 0400, 3/28/79 63 2 LLAle Kl-,yeIWpn1 DIKROFZ PLOT e 3

0 UDRbS 3033 TDTAL ERRS 0

ws ROUGH DRAn

30UG3 D3 AFT

.e P

MODIFIED AREAS, RHOS, CORRECT PRZR. COMP.PP. SOL 1.600 '

i i

i i.

i i

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+

3*

1.400 -

1.200

~

racssN' WORK

~

1.000

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=

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=

0.000

- 2000 i

0 00 50.0

100, 150.

200.

250.

300.

HOURS AFTER 0400, 3/28/79 Fy 3

pubble Volama al 875 sts f

ROJGE D3AF,

ROUG3 DRAF MODIFIED AREAS, RHOS, CORRECT PRZR, COMP,PP. SOL 200.0 180.0'-

160.0 140.0

\\.

?RG$EWT YORC

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er 120.0

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100.0

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80.00 i

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mo

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20.00 0.000 O.00 50.0 100.

150.

200.

250.

300.

HOURS AFTER 0400, 3/28/79 F)l TbM f 6 n,a Rcs q

ROUGH DRAF l

9 P

gr

o R.K. Cola,Jr.

S:ndia Lab;, Albuquezqua N.M 15 october 1979 c.

HTDROGEN BURN The attached graph was constructed assuming a containment atmosphere initia13v saturated with water at a temperature of 1200F at a slight 4

overpressure of 15 psig relative to atmospheric pressure of 14 3 psia. It shows that an overpressure of 26 to 28 psig requires an initial hydrogen concentration of 7.I to 7.4%.

If the containment building volume is taken as 2.05x106 3

fg, we find that this requires 16fto ISO kg moles (330 to yoO kg). The burn will produce a 16f to IEO kg moles of water in addition to the initial 250 kg moles, and the post-burn atmosphere will have few point near 14foF. Therefore, we feel (but have not shown conclusively) that the primary mechanism for

[

pressure decay is cooling Icf evaporatio of additional water.

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