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U. S. ATOMIC ENERGY C O M M I S S I O N

ORNL- TMcow
DATE

No.

6 6 $J 67

- October 18, 1g61

Buildup of F i s s i o n Products i n Reactor Fuel and Coolant with 'Unclad ' Fuel Material
Wrn. B. C o t t r e l l and L. A. Mann

Abstract Concentrations of f i s s i o n products i n t h e f u e l and i n t h e coolant stream of a generalized reactor power p l a n t employing unclad f u e l material have been calculated using a c t u a l f i s s i o n ) product chains and wide ranges of assumed values of 1 escape r a t e from t h e f u e l and 2) removal r a t e from t h e coolant stream. The calculations were made on an IBM 704 d i g i t a l computer. Some t y p i c a l r e s u l t s a r e displayed i n t h e form of graphs t o i l l u s t r a t e t h e e f f e c t s of t h e v a r i a b l e s . The complete t a b l e s of calculated d a t a a r e available but a r e not included with t h e present report. As d a t a on escape r a t e s from f u e l and removal r a t e s from coolant become available, t h e t a b l e s and graphs developed by t h i s study can be used t o estimate t h e fission-product concentration i n t h e coolant stream, which would i n t u r n f u r n i s h a b a s i s f o r determining t h e degree of coolant p u r i f i c a t i o n required t o maintain t h e c i r c u l a t i n g a c t i v i t y below a given l e v e l .

*We L. Albrecht of TVA p a r t i c i p a t e d i n t h e formulation of t h i s study before being subsequently reassigned.

NOTICE
T h i s document contains information o f a preliminary nature and was prepared p r i m a r i l y for i n t e r n a l u s e at the Oak Ridge N a t i o n a l Laboratory. It i s subject The t o r e v i s i o n or correction and therefore does n o t represent a f i n a l report. information i s n o t t o be abstracted, reprinted or otherwise g i v e n p u b l i c d i s seminotion without the approval of the O R N L patent branch, L e g a l and Infor-

L E G A L NOTICE T h i s report wos prepared as an account of Government sponsored work. nor the Commission, nor any person acting o n behalf of the Commission: A. Makes any any warranty or representation, expressed or implied, w i t h respect t o the accuracy, or usefulness of the information contained i n t h i s report, or that the use of apparatus, method, or procass d i s c l o s e d i n t h i s raport may not i n f r i n g e completanass, Neither the United Stoles,

information,

p r i v o t a l y ownad rights; or

B . Assumes any l i a b i l i t i e s w i t h raspact t o the us- of, or for damages r e s u l t i n g from the usa o f
any information, apparatus, method, or process d i s c l o s e d i n t h i s raport. As used i n the abova, "person a c t i n g o n behalf of the Commission" includes any employes or

controctor or

of the Commission, or amployaa of such contractor, t o the extant that such amployee of tha Commission. or amployee of such contractor prepares, dissaminatas, or

contractor

provides access to, any information pursuant t o h i s employmant or contract w i t h the Commission, or h i s amploymant w i t h such contractor.

Table of Contents Page

Introduction

......................... 6 F i s s i o n - P r o d u c t Escape from F u e l . . . . . . . . . . . . 6 F i s s i o n - P r o d u c t F a t e i n t h e Coolant . . . . . . . . . . . 7

Range of Parameters Examined

. . . . . . . . . . . . . .

Mathematical A n a l y s i s

....................

1 1

Summary of t h e D i f f e r e n t i a l Equations f o r a Four-Membered Chain D e r i v a t i o n of t h e S o l u t i o n s t o t h e D i f f e r e n t i a l Equations S o l u t i o n of a Chain Three Members o r Less Nomenclature f o r Mathematical Analysis

.................. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .........

1 1

15 16
17

Results

. . . . . . . . . . . . . . . . . . . . . . . . . . .

18 27
27

Discussion

. . . . . . . . . . . . . . . . . . . . . . . . . . I n h a l a t i o n Exposures . . . . . . . . . . . . . . . . . . DirectRadiation . . . . . . . . . . . . . . . . . . . . E f f e c t of Removal Rate on Concentration i n Gas . . . . . E f f e c t o f D ' on Concentration i n Gas . . . . . . . . . . Some C o n s i d e r a t i o n s i n D ' v s Ng R e l a t i o n s . . . . . . . .

28 29
30 30

Conclusions and Recommendations Appendix A . Appendix B . Tables

...............

33
35

Eucl.ear P r o p e r t i e s of Fission-Product I s o t o p e s Arrangement and Use of t h e IBM 704 Print-Out

..

. . . . . . . . . . . . . . . . . . . . . . . . . I n p u t Data . . . . . . . . . . . . . . . . . . . . . . . Computer P r i n t - O u t Table Headings . . . . . . . . . . . .

40 40 40 40 41

I n d i v i d u a l I s o t o p e s ~ Case I . . . . . . . . . . . . . . 1 Cases I1 and 1 1 I s o t o p e Tables Nuclide Sums. A l l Cases

................

............

41
43
45

Ai. pendix C Arrangement and Use of Proposed T a b l e s of ComputerOutput

..................... References . . . . . . . . . . . . . . . . . . . . . . . . . . Figures . . . . . . . . . . . . . . . . . . . . . . . . . . . .

46

-3L i s t o f Tables Page F i s s i o n Product Elements Included i n t h i s Analysis. S e l e c t e d Constants o f S i g n i f i c a n t I s o t o p e s f o r P o t e n t i a l I n t e r n a l Exposure. Gas Concentrations and R e l a t i v e I n t e r n a l Hazard P o t e n t i a l of S e l e c t e d I s o t o p e s f o r Various Values of' D' and r. S e l e c t e d Constants of I s o t o p e s S e l e c t e d f o r D i r e c t R a d i a t i o n Exposure P o t e n t i a l
G a s Concentrations and R e l a t i v e D i r e c t R a d i a t i o n Hazard P o t e n t i a l of S e l e c t e d I s o t o p e s f o r Various Values of D' and r

Tab1e No. 1

1-9

Amounts of sr90 i n Gas from ~b~~ Decay D and ~ r 9 O i f f u s i o n I l l u s t r a t i o n s of Use of Sums Tables f o r Cases I1 and I11 Concentrations o f I n d i v i d u a l I s o t o p e s i n Gas ( c a s e I )

L i s t of Figures
A l l f i g u r e s a r e p l o t s of t h e "Buildup of F i s s i o n Products i n Coolant." The information l i s t e d a f t e r the f i g u r e number i n t h e l i s t below i s the s p e c i f i c isotope and conditions i n each case.

Figure 1. Figure 2 . Figure

r Case I, ~ l =, ~ D

r = 0 t o 1 ( s e c- ) . 1

- 2 1 JSr 87, Case I, D ' = 1 0 , r = 0 t o 1 ( s e c-1) *

3.

S r89, Case I, D 1 =

r = 0 t o 1 (sec'l).

Figure 4. Figure Figure Figure

) Sr89, Case I, D 1 = 10-12 r = 0 t o 1 ( s e c 1 .

sr90, Case I, D ' =

5.

6.
7.

srgo, Case I, D '

r = 0 t o 1 (sec-l).
-10 10

sr90, Case I, D' = sr90, Case 1 , D ' 1 a

,r 1 0-12 , r
=

= 0 t o 1 (sec = 0 t o 1 (sec

-1

). )

-1

Figure 8. Figure

r = 0 t o 1 (sec'l).

9.

Figure 1 0 . Figure 1 . 1 Figure 1 2 . Figure Figure

- 2 1 1 , D 1 = 10 1 , r = 0 t o 1 (sec-l). a 1 sr90, Case 1 1 D ' = 1, r = 0 t o 1 ( s e c- ) a srgO,Case 111, D l a = 10-10 , r = 0 t o 1 ( s e c-1 . )

srgO,Case

sr90J Case 1 1 D ' 1, y90, Case I, D l =

= 10'12,

r = 0 t o 1 (sec'l).
a

13.
14.

1 r = 0 t o 1 ( s e c- )

-2 1 y90, Case I, D ' = 1 0 , r = 0 t o 1 ( s e c-1)

Figure 1 5 . Figure Figure

1 3, Case I, D 1 = 1 '
lL3', Case I, D l = 1 0

1 r = 0 t o 1 ( s e c- ) . -12

16.
17.

,r

0 t o 1 (sec

1
) a

11j4, Case I, D l =

r = 0 t o 1 (sec

-1

).

Figure 18. Figure

Case I, D l = 10'12,

1 r = 0 t o 1 ( s e c- )

19.

I~~~~ Case I, Dl =
-12 11S5, Case I, D ' = 10 Case I, D ' = cs1j8, Bal4', -1 2 Case I, D ' = 10 Case I, D l =

r = 0 t o 1 (sec-l)

.
)*

Figure 20. Figure 21. Figure 22. Figure 2 J .

,r

0 t o 1 (sec

r = 0 t o 1 ( s e c -1)

,r

= 0 to

1 (sec

r = 0 t o 1 (sec

).

Figure 24. Figure 25. Figure 26. Figure 27. Figure 28. Figure 29. Figure 30. Figure 31. Figure 32. Figure

-12 1 a Case I, D~ = 1 ~ ~ ' 0 ,r = 0 t o 1 ( s e c ) .

La140, Case I, D ' =

lom7, r

= 0 t o 1 (sec-l).

La140, Case I, D 1 = 10-lo, r = 0 t o 1 ( s e c La140, Case I, La140,

Dl

1 1

.
)

10-12, r = 0 t o 1 ( s e c
=

).

Case 11,

D l a

r = 0 t o 1 (sec
-12 , -10 -2 1

-1

La140, Case 11, D 1 = l O a ~ La140, La140, 144 Ce a Case 1 1~ D l a ~ ~ 1, = Case 1 1 1 ,

Dla

,r
r

= =

0 t o 1 (sec-l) . 0 t o 1 (sec-l).
-1

= 10

r = 0 t o 1 (sec
=

).
)

Case 1 1 D l a = 1 0 1,

,r

0 t o 1 (sec

-1

33.

Figure 34. Figure 35. Figure

, Case 144, Case Ce

Pr
144

I, D

r = 0 t o 1 (sec-l).
1

I, D ' = 10-12, r = 0 t o 1 ( s e c
=

144, Case I, D ' Pr

lom7,
- 2 1

r = 0 t o 1 ( s e e-1 . )
= O t o 1 (sec
1

36.

, Case

I, D ' = 1 0

,r

).

Introduction

This study i s d i r e c t e d toward p r e d i c t i n g t h e b u i l d u p of c o n c e n t r a t i o n of f i s s i o n - p r o d u c t a c t i v i t y i n a gas-cooled power r e a c t o r coolant stream a s a f u n c t i o n of time, fission-product escape r a t e s and removal r a t e . t h e purposes of t h i s study, all removal processes i n c l u d i n g d e p o s i t i o n , leakage, and p u r i f i c a t i o n have been considered t o g e t h e r a s t h e removal rate, For

A c o r o l l a r y study would be t h e determination of t h e d i s t r i b u t i o n of

deposited a c t i v i t y i n a coolant system when s u f f i c i e n t d a t a on d e p o s i t i o n become a v a i l a b l e . The problem of coolant a c t i v i t y i s a general one f o r power r e a c t o r s u s i n g e i t h e r c l a d o r coated s o l i d f u e l s , s i n c e a l l power r e a c t o r s depend on coolant flow t o remove t h e h e a t of f i s s i o n and decay and s i n c e t h e p r o b a b i l i t y always e x i s t s t h a t f i s s i o n products w i l l e n t e r t h e coolant stream v i a imperfections i n t h e f u e l c o a t i n g o r cladding. The same

t h e o r y and c a l c u l a t i o n a l methods used h e r e could be a p p l i e d t o l i q u i d cooled r e a c t o r s with a p p r o p r i a t e l y chosen ranges of removal r a t e parameters. The l e v e l of a c t i v i t y i n t h e coolant gas w i l l be important t o t h e det e r m i n a t i o n of t h e hazards of r o u t i n e and a c c i d e n t a l r e l e a s e s of t h e primary coolant. The c o s t and d i f f i c u l t y of maintaining t h e coolant sysI n t h i s study, t h e d e p o s i t e d

tem w i l l depend l a r g e l y on t h e l o c a t i o n s and amounts of deposited a c t i v i t y , which t h i s study does not attempt t o analyze. c l e a n i n g methods a r e used (e.g., a c t i v i t y i s combined with t h a t removed from t h e coolant by whatever a f i l t e r i n a by-pass system) and t h e t o t a l removal r a t e t h u s obtained i s designated by t h e symbol r ( f r a c t i o n removed per second)

However, t h i s does permit t h e d e t e r m i n a t i o n of p u r i f i c a t i o n

system requirements t o o b t a i n a cooling system concentra3ion of a c t i v i t y l e s s t h a n any given value, i f indeed a p u r i f i c a t i o n system i s needed a t all. Fission-Product Escape from Fuel The escape of f i s s i o n products f r 0 m . a f u e l element i s t a k e n h e r e t o be a d i f f u s i o n a l process, f i r s t i n d i f f u s i o n t o t h e s u r f a c e o f t h e p a r t i c l e o r c r y s t a l i n which t h e f i s s i o n occurred, t h e n o u t through t h e f u e l element

matrix t o i t s surface, where it i s assumed t h a t t h e atoms of f i s s i o n products e n t e r the flowing gas coolant stream through a d e f e c t i v e o r porous f u e l container o r coating. This a n a l y s i s assumes t h a t t h e d i f f u s i o n of t h e f i s s i o n products i s c o n t r o l l e d by t h e f u e l p a r t i c l e and not by t h e processes by which it i s subsequently released t o t h e coolant stream. For an element c o n s i s t i n g of UO p a r t i c l e s i n a graphite matrix, t h e 2 d i f f u s i o n t o t h e s u r f a c e of t h e UO p a r t i c l e i s indeed controlling.' For 2 o t h e r types of f u e l element, d i f f u s i o n through t h e matrix m y be more s i g n i f i c a n t o r even c o n t r o l l i n g ( f o r example, UO particles i n a stainless 2 s t e e l matrix coated i n t u r n by a s t a i n l e s s s t e e l s h e a t h ) . Since t h e s i z e s

and shapes of f u e l p a r t i c l e s and t h e escape r o u t e s from f u e l p a r t i c l e s t o t h e f u e l element surface vary t o a degree t h a t has so f a r prevented use of t h e a c t u a l d i f f u s i o n c o e f f i c i e n t s (where known), experimental " v i r t u a l " d i f f u s i o n c o e f f i c i e n t s ( D ' ) have been employed. 2'3 Eichenberg, e t a l . , 2 and i s surm~arizedby C o t t r e l l , e t a1.l parent o r disappear by decay t o i t s daughter. generations a r e considered i n t h i s a n a l y s i s . This r e p o r t i s not intended t o be s p e c i f i c a s t o what numericaL values of
Dl

The theory

of t h e escape process i n s i d e t h e f u e l element i s explained i n d e t a i l by Alternatively, an isotope may form within t h e f u e l element o r t h e gas by decay of i t s Decay chains of up t o f o u r

and V (escape parameters defined i n t h e s e c t i o n on a n a l y s i s )

should be expected t o be v a l i d f o r isotope escape from f u e l , b u t covers the range 1 0

-14 t o l o m 7 f r a c t i o n removed per second because some experiments 4 ~ 5

i n d i c a t e t h a t t h e value may eventually be found t o be within t h a t range a t f u e l element temperatures of most i n t e r e s t . Fission-Product F a t e i n t h e Coolant When a r a d i o a c t i v e isotope e n t e r s t h e coolant stream it may decay, deposit on a container surface, l e a k out, be removed by a chemical o r physical process ( e . g . , stream. a f i l t e r ) , o r remain suspended i n t h e f l u i d

It i s assumed here t h a t no isotopes move from t h e f l u i d stream

i n t o the fuel.

This r e p o r t makes no attempt t o specify t h e a c t u a l means of removal from t h e coolant but covers t h e range r = 0 t o r = 1 of removal r a t e s , where r = f r a c t i o n removed per s e c by a l l processes combined except r a d i o a c t i v e

decay which i s included s e p a r a t e l y and i s considered i n m r i a ~ t ? ;On. t h e o t h e r hand d e p o s i t i o n , leakage and p u r i f i c a t i o n a r e o r may be s u b j e c t t o c o n t r o l . Deposition on a c o n t a i n e r s u r f a c e i s c o n t r o l l a b l e t o some e x t e n t by design o r m a t e r i a l s p e c i f i c a t i o n although t h e r e may be some p r a c t i c a l l i m i t a t i o n s on t h i s process. Nornal leakage from t h e coolant system can be c o n t r o l l e d

by design and maintenance s p e c i f i c a t i o n s , whereas removal by chemical o r physical processing may be e f f e c t e d e i t h e r i n t h e main coolant stream o r , more u s u a l l y J i n a bypass c i r c u i t . Some

test^^'^

indicate t h a t deposition

i s sometimes much more dependent on chemisorption t h a n on condensation o r

physical ( e . g . , van d e r waals) a d s o r p t i o n ,

It i s hoped t h a t t h e range o f

t h e removal r a t e ( r ) s e l e c t e d f o r use i n t h i s study w i l l be anenable t o i n t e r p o l a t i o n t o experimental v a l u e s . The removal r a t e s used h e r e r e p r e s e n t t h e sums of t h e removal c o n s t a n t s f o r leakage, d e p o s i t i o n and purification. Not only i s it n o t now p o s s i b l e t o s e p a r a t e deposited a c t i v i t y from t h a t removed by o t h e r processes, b u t a l s o t h e l a c k of e i t h e r d a t a o r accepted t h e o r y prevents determination of t h e d i s t r i b u t i o n of d e p o s i t e d r a d i o a c t i v e i s o t o p e s i n t h e coolant system,

It has become evident 778 t h a t

d e p o s i t i o n b y condensation of f i s s i o n products from t h e coolant caused by exceeding t h e s a t u r a t i o n c o n c e n t r a t i o n i n t h e coolant i s f r e q u e n t l y comp l e t e l y i n v a l i d a s a b a s i s f o r p r e d i c t i n g removal r a t e s o r d e p o s i t i o n locations. Study and t e s t i n g of o t h e r f a c t o r s (such as chemisorption, van d e r Waals adsorption, e t c . ) which i n f l u e n c e t h e removal of f i s s i o n products i s a t an ea.rly s t a g e of development. Range of Parameters Examined The b a s i c parameters considered i n t h i s study a r e 1) t h o s e a f f e c t i n g r a t e s of d i f f u s i o n from, t h e f u e l elements ( D ' ) , and 2 ) t h e assumed, removal ra.tes ( r ) from t h e coolant, and 3) o p e r a t i n g time ( t ) .
Dl

(see'')

may be defined a s a constant times t h e amount of an i s o t o p e

2

d i f f u s i n g out per second evaluated a t t h e s u r f a c e of t h e f u e l p a r t i c l e ,

It a r i s e s from a t h e o r e t i c a l d e r i v a t i o n

a s an experimentally determinable

value f o r a p a r t i c u l a r s e t of c o n d i t i o n s .

D'

/ ( a e c~ ), where D s

i s t h e conventional d i f f u s i o n c o e f f i c i e n t (cm / s e e ) and a i s a c h a r a c t e r i s t i c l e n g t h 2 a s s o c i a t e d with t h e f u e l (cm), such a s t h e r a d i u s i n t h e case of a

spherical fuel p a r t i c l e . Three "cases" were included i n t h e c a l c u l a t i o n s of both t h e elements and the isotopes, a s follows. Case -- I. sec-'. Case --11. value of I n the Case I1 c a l c u l a t i o n s t h e value of D f ( = I n t h e Case I calculations, the value of D' (=D;

) used i s

the same f o r every element, over t h e range of values D' = 10-12to D I =

) used

f o r elements of atomic numbers 35-37 and 51-55 i n c l u s i v e i s 10-1 times t h e

Dl

( = Da ) f o r t h e o t h e r elements i n Table I over t h e range '

sec-l. The reason i s explained below.

D' = 1 0 - l 3 t o D' = Case 11 --1.

I n t h e Case I 1 c a l c u l a t i o n s t h e value of D' (= Dh ) used 1 2 times th.e f o r elements of atomic nmbers 35-37 and 51-55 i n c l u s i v e i s 10

value of D l ( = D i ) f o r t h e o t h e r elements i n Table I . explained below. thus 10-l4o t The t o t a l range of

Dl

The reason i s

covered f o r t h e s e elements i s 1

10-7 s e c - l .
Cottrell, e t a l . , reported t h a t experi
Dl

Reason ----f o r Cases I1 and 1 1 1 . mental d a t a show t h a t t h e

values f o r some elements a r e s i g n i f i c a n t l y

d i f f e r e n t from others a t t h e same temperatures (pp

76-81, ORNL-2935). The

Therefore,

evidence i s not c l e a r a s t o the q u a n t i t a t i v e r e l a t i o n s , but it appears t h a t f a c t o r s of d i f f e r e n c e of a t l e a s t up t o 100 a r e involved. t h i s a n a l y s i s assumed t h e factor's of d i f f e r e n c e l i s t e d above f o r t h e Case I1 and Case I11 c a l c u l a t i o n s .

It should be emphasized t h a t t h e
As

s e l e c t i o n s a r e i l l u s t r a t i v e , not q u a n t i t a t i v e , and t h a t experiments m y show t h e f a c t o r s of difference t o be o f f by orders of magnitude. experimental values accumulate, values within t h e ranges s e l e c t e d m y be used f o r i n t e r p o l a t i o n , while values outside t h e s e l e c t e d ranges may be used a s input d a t a f o r new c a l c u l a t i o n s . The parameter r ( s e c - l ) i s t h e f r a c t i o n a l r a t e of disappearance from t h e coolant stream, t h a t i s , it i s t h e f r a c t i o n of t h e t o t a l invent o r y of t h e isotope i n t h e coolant which disappears from t h e coolant per second. cation. This parameter incl.udes l o s s by leakage, deposition, and puri f i Values of r s e l e c t e d f o r t h i s study range all t h e way from zero The same values of r were used i n each of

t o one, and were chosen with t h e i n t e n t of permitting i n t e r p o l a t i o n between the values s e l e c t e d . t h e t h r e e cases studied.

The parameter of time ( t ) i s given i n seconds a f t e r r e a c t o r s t a r t u p .

It i s assum.ed t h a t s t a r t u p i s i n s t a n t a n e o u s and t h a t o p e r a t i o n i s s t e a d y
s t a t e t o t h e time i n question. The range of values of t used was from 1 05 seconds (approximately 28 hours) t o 1 0

8 seconds (approximately 3.2 y e a r s ) ,

t o cover t h e range from reasonably s h o r t o p e r a t i n g times t o times l o n g enough t o be a t o r n e a r e q u i l i b r i u n c o n c e n t r a t i o n s of most f i s s i o n product s .

Mathematical A n a l y s i s Using t h e b a s i c parameters d e f i n e d above and t h e b a s i c r a d i o a c t i v e decay parameters, t h e g e n e r a l i z e d system was a n a l y z e d mathematically by

J . Replogle o f C e n t r a l Data Processing, ORGDP.

C e n t r a l Data P r o c e s s i n g . The a n a l y s i s f o l l o w s .

C a l c u l a t i o n s were performed

on a n IBM 704 d i g i t a l computer u s i n g a program w r i t t e n by J. L. Lucius o f Only t h e parameters used throughout t h e a n a l y s i s a r e d e f i n e d i n t h e Nomenclature, page needed. 17. Other c o n s t a n t s and parameters a r e d e f i n e d as

The a n a l y s i s i s f o r a four-membered decay c h a i n and r e s u l t s i n

e q u a t i o n s d e f i n i n g t h e e x i s t i n g amount o f each i s o t o p e a s a f u n c t i o n of time i n b o t h t h e f u e l and t h e gas c o o l a n t . The c a l c u l a t e d amounts were p r i n t e d o u t as t h e number o f atoms of i s o t o p e p e r f i s s i o n p e r second i n t h e f u e l elements l e a k i n g t o t h e c o o l a n t .

I.

Summary of t h e D i f f e r e n t i a l Equations f o r a Four-Membered Chain

A.

F i s s i o n product i n t h e f u e l .

where,

-12-

F = ~ ( t ) the fraction of an isotope in the gas, of the total in is

both the gas and the fuel at the time under considerationY The solution to this system is;

where A1 A2 As Ah As A6 A
= = =
= = =

A a, +V a Ab+vb
6Aa y,/q
(yb
+

Aj)/A2

c
+V

q)

=
=

A4hb Ughb

A8 A9 A10 All
A12

= = = =

(A7

Y,)/A~

-~7)
(A6
91

- A2)

A1O

B. F i s s i o n Products i n t h e gas ( c o o l a n t ) .

where Nd
Ndl
=

Ndl g

Nd2

'

1 1 atoms f i s s i o n- s e c -

= =

amount i n t h e gas which had d i f f u s e d out from t h e f u e l amount i n t h e gas which appeared from decay of i t s parent which was a l r e a d y i n t h e gas

N~~~

The s o l u t i o n t o t h i s system. i s :

where

and r

fractional rate of disappearance from suspension in gas (assumed constant), sec-1

11. Derivation of t h e Solutions t o t h e D i f f e r e n t i a l Equations

The ' f i r s t t h r e e equations of a four-membered chain a r e solved by LaPlace transforms.

he ' l a s t equation f o r t h e f u e l can be w r i t t e n a s :

2+ dt
IShose s o l u t i o n i s :

A (t)x

B (t)

x
where

= e-Jiidt

J ( elAdt ) mt + c e -J ~

d t

constant t o be valuated from t h e condition x ( 0 ) = Q i s solved by transposing t h e term However, t h i s l e a v e s t h e

The d i f f e r e n t i a l equation f o r Nd2'

r N ~ ~ o ' t h e l e f t s i d e of t h e equation and applying t h e operator t

0

it

erT dT t o both s i d e s of t h e equation.

integrd

ol e

r 7

Ndf

(T)

F (T ) d T

t o be e ~ l U a t e d numerically, and

considerable c a r e must be taken t o avoid round-off e r r o r s i n the

machine c a l c u l a t i o n s .

The form of t h e s o l u t i o n t h a t was found t o be

t r a c t a b l e i n all b u t a few cases i s a s follows:

:N

(t) m) ( t ) + M ( t ) + r e -rt
K

I.

E m
(t)

where

K (t) =

e -'t
0

err P1

(T)

dr The l a t t e r functions a r e e a s i l y

and M ( t ) has been defined previously.

evaluated a s they a r e l i n e a r i n t and exponentials of t . The i n t e g r a l was evaluated by t h e generalized mean value theorem k by estimating 7 i n each of 2 equal s u b i n t e r v a l s . The i n t e g r a l i s then:
j

with

to = 0
and

(2

= t

111. Solution of a Chain of Three Members o r Less.

Each member of t h e chain i s solved according t o i t s c h a r a c t e r i s t i c -1 1 d e s c r i p t i o n i n t h e chain except f o r isotopes with h < 10 I n t h i s case

t h e equation i s solved a s i f t h e isotope were s t a b l e a s represented by t h e f and N : i n P a r t I, with Ncf and Ncg being replaced by equations f o r N d t h e next higher element i n t h e chain.

Nomenclature for Mathematic'aJAnalvsis

nuniber of ato~nsin fuel (or gas) at ' i e t after cn startup

fractional rate of disappearance from suspension in -1 gas (assumed constant), sec fission yield, atoms of species appearing per fission, -1 fiss fraction of y which is isomer being calculated fractional decay rate, sec
-I

= = =

fractional rate of disappearance from the fuel matrix (assumed constant),

V

3 J h ~ ' (see ref. 2, Ee;. V-10)

Superscripts f
= =

fuel gas

e;

Subscripts a,b,c,d
=

member of d.ec~y chain a

-+

-+

-+

A s s t a t e d above, t h e c a l c u l a t i o n s i n t h i s study apply only t o those

f u e l elements which o f f e r no r e s i s t a n c e t o t h e escape of f i s s i o n products from t h e f u e l material surface t o t h e coolant gas.

The t a b u l a t e d r e s u l t s

have t h e u n i t s " t o t a l number of atoms per f i s s i o n per second" f o r concent r a t i o n s i n both uncontained f u e l elements and i n t h e coolant gas a t t h e l i s t e d values of D', r, and time of continuous s t e a d y - s t a t e operation since r e a c t o r s t a r t u p . Results were c a l c u l a t e d f o r t h e elements l i s t e d i n Table 1 and f o r t h e isotopes and isomers l i s t e d i n Appendix A. Table 1 with atomic mass numbers 85 through included i n t h e c a l c u l a t i o n s . Nuclides of t h e elements i n

106

and 127 through 1 5 1 were

This includes a l l isotopes of t h e l i g h t

i

(groups A ) elements form rubidium through molybdenum, and of t h e heavier (group B) elements form iodine through pmlhethium, plus t h e more s i g n i f i c a n t isotopes of t h e o t h e r fission-product elements. The a c t u a l concentrations may be obtained from t h e r e l a t i o n s :

and

w i t h t h e nomenclature: concentration of nuclide i, atoms c -3 m

'i

f i s s i o n power generated i n t h e l e a k i n g f u e l elements, 1 f i s s i o n s sec t o t a l atoms of nuclide I i n t h e medium s p e c i f i e d , 1 1 atoms f i s s i o n sec volume of t h e medium s p e c i f i e d , c 3 m

Ni
v

Table 1. Fission-Product Elements Included in this ilnalysis

Group A
( Lighter Elements )
Element Br Atomic l o d. (Heavier Elements ) Element Atomic No.

Kr
Rb

Sr

Y
Zr
ND

bo l Tc

Ru Rh
Pd

I n a s much a s it was not p r a c t i c a l t o include all t h e d a t a f o r all i s o t o p e s f o r all t h e cases, 1 2 isotopes were s e l e c t e d from Appendix A f o r i l l u s t r a t i v e treatment. They were chosen roughly on t h e b a s i s of

combinations of f i s s i o n yield, decay constant, b e t a o r gamma energy, and b i o l o g i c a l significance.'' They a r e not intended t o be i n c l u s i v e , but and r, on t h e hazards and t h e r e f o r e on t h e The 1 2 i s o t o p e s

they were chosen only a s s i g n i f i c a n t examples t o i l l u s t r a t e t h e e f f e c t s of t h e parameters time,

Dl,

design s p e c i f i c a t i o n s of f u e l and coolant systems. s e l e c t e d were K I - ~ ~Sr8', ,

srgO,ygO,

1 3 ,I 1 1

~ I~~~~ ~ ~

, Ba14'

La1407

1 4 4, a n d P r144 . Ce
Some of t h e e f f e c t s of t h e parameters of time,
Dl,

and r, on t h e con-

c e n t r a t i o n s of t h e 1 2 isotopes chosen a r e shown i n F i g s . 1 through a r e presented f o r convenience a t t h e end of t h e r e p o r t . graphs of Ng ( t o t a l atoms i n t h e g a s / f i s s / s e c )

36 which

Included a r e

f o r Case I f o r all 1 2

' i s o t o p e s and of Ng f o r Cases I1 and I11 f o r t h e long-lived (28-yr) S r9 and t h e r e l a t i v e l y s h o r t - l i v e d La14' (whose N g depends e s s e n t i a l l y on
t h e decay of 1 2 . 8 day Ba14'). For t h e time s c a l e used, concentrations of t h e r e l a t i v e s h o r t - l i v e d i s o t o p e s which a r e not daughters of long-lived precursors appear a s e s s e n t i a l l y s t r a i g h t h o r i z o n t a l l i n e s . This would

n a t u r a l l y be expected, because of t h e more r a p i d approach t o equilibrium concentration a s t h e h a l f - l i f e becomes s h o r t e r . I n a d d i t i o n t o t h e r e s u l t s shown i n Figures have been analyzed on one of two bases,

1-36, s e l e c t e d isotopes

1) those which c o n s t i t u t e t h e
The s e l e c t e d i s o t o p e s i n

more serious, p o t e n t i a l i n h a l a t i o n exposures, and 2 ) those which c o n s t i t u t e t h e more s e r i o u s d i r e c t r a d i a t i o n p o t e n t i a l . each group a r e t a b u l a t e d i n Table 2 and

4 respectively, t o g e t h e r with

nuclear o r b i o l o g i c a l constants which describe t h e r e l a t i v e p o t e n t i a l of each. Table

3 then l i s t s t h e concentration of isotope given i n Table 2

Likewise, Table 5 l i s t s t h e

f o r a number of values of D' and r, together, i n all instances, with t h e index of t h e i n h a l a t i o n hazard p o t e n t i a l .

concentration of t h e isotopes given i n Table of

Dl

4 f o r a number of conditions

and r, t o g e t h e r i n all instances, with an index of t h e d i r e c t

r a d i a t i o n hazard p o t e n t i a l .

Table 2. Selected Constants of S i g n i f i c a n t Isotopes f o r P o t e n t i a l I n t e r n a l Exposure

TID( ')/NP

Isotope

a 8 Taken a t 1 0 s e c a f t e r s t a r t u p with steady operation a t 100 M w t . b ~ h i s i s a f a c t o r t o convert pc t o mrem T I D . It i s not a d i f D f u s i o n parameter. The values of D have been corrected from r e f . 1 0 by using d a t a i n t h e ICRP Committee I1 Report (1959)TID f o r i n h a l a t i o n of - t h e coolant ( t o be m u l t i p l i e d by t h e all f r a c t i o n of f u e l elements l e a k i n g - by t h e f r a c t i o n of leaked atoms and inhaled).
C

L n

t
L n L n

r l r l r l r l r l

X
c - ; L n t -

X
\O

X
rl
rl 0 0 rl X C I U 0 0 rl X

rl X rl

4
X X X
L n

r l r l r l c u c u

. ? ?
0

.
l
0 0 0
I 0

0 0 0 0 0 r l r l r l r l r l X X X X X
0

L n \ O
Ln Ln

0 rl

o
0 0 0 0 0 r l r l r l r l r l X X X X X

o
1

o
r l r l r l r l r l X X X X X
rl X
0 rl. X

'

U l

M 1 0

t l = ? = ? ?
M A Q r l t Q

= !
CU

?
rl

r l r l r l r l r l X X X X X

h
X
rl

o
C U r l r l M r -

.y

rl X

a*

1 %
CU

C U C U C U 0 0 O - b r l O

r l r l r l r l r l X X X X X

CU 0 rl X

CU. 0

rl X X X

O O T ; ' ? ? 0 0 0 0 0 r l r l r l r l r l

0 0 rl X

rl

0 rl

rl 0

r l r l r l o o -b -'o d o
0

r l r l r l r l r l X X X X X

-'o
rl X
rl X

CU 0

r l r l r l r l r l X X X X X

Q 0

m .
rl X
0

rl X

r
r l r

l \

0
D

q ?
\ O M

r-

r! "0.
CU

A 0 rl X

A M 0 0 rl rl X X

C U 0 0 rl rl X X

f A 0 rl X

0 rl X

CU 0 0 0 0 0 " r l r l r l r l r l X X X X X

T;'

CU 0 rl X

CU 0

rl
X

d o

r l r l r l r l r l X X X X X

-'o

- C U O rl rl 0 0

-'o

rl 0

r l r l r l r l r l X X X X X

0 rl 0

r-

Q 0

cn

0 0

rl X

d o

rl #

L n r - A -

r l r l r l r l r l X X X X X
" ? O ?

odo

CU 0

M 0

A-

r l r l r l r l r l

odo

T;' 0
C U A r l A r n

0 0

CU 0

-3-

X
\ O ? M C U C U m r r

X
J l r

X
g l

rl X

0 "

rl X

"0.
V

qM
K\.

0\

m Q

?
m
k

A rlH

0 0 A-A-

II

Ln

4t-I

A-A *ArlH

'd d ~9 A

rlg-2

X
C O c O L n O

X
"
M

X
O
L n

X
"
r

X
?
i r i

X
M

X
C

X
U

? " - ' , ?
M

Table

4.

S e l e c t e d Constants of Isotopes S e l e c t e d f o r Direct Radiation Exposure P o t e n t i a l

Total(b) E (Mev/ii s )

a 8 Calculated f o r 1 0 sec a f t e r s t a r t u p ; steady-operation a t 100 M w t .

b ~ o g r e a t e r refinement of accuracy, use E s e p a r a t e l y f o r each r g energy group and u l t i p l y N by f r a c t i o n i n theyenergy group, then 0 Ng C Eii A . f r a c t i o n , s i n c e t h e hazard i s high f o r sum t h e 3.1 x 1 ' 1 harder gammas f o r t h e same ~ e v / s e c . T o t a l a c t i v i t y i s - t h e coolant. The concentration and geometry all w i l l determine t h e hazards. Also see note b.
C

Table 5.

Gas Concentrations and Relative D i r e c t Radiation Hazard P o t e n t i a l of S e l e c t e d Isotopes f o r Various Values of D' and r

D' = D i

Dd
=

lom7

. ,

1 08 s e c

Case I
K r 87

Activity atoms/(fiss/sec) ( ~ e v / s e c ) / 1 0 0Mwt

Ng

10

-6
Ng

= 10 4
Activity

10

-2

Ng

Activity

Ng

Activity

,131 ,134 ,135 C s138

Ba La 140

140 144 Ce 144

Pr
I)'= D a
=

D ;

lo-1z

1 08 s e c

-I= . d

h r l r l r l r l 0 0 0 0 rlrlrlrl
X X X X
0 0 0 0 r l r l r l r l X X X X

r l C U O C U

m r l c o r l

y
0

"
CU,-!Fi<
0 C - c o C U
r l C U M r l 0 3
1 1 1
L n

. d -I= 0

b-

CUP-r-9
1

. .

11

k
0

7 9 0 0 0 0 rl rl rl 0 rl 0 0 0 rlrlrlrl
1

CU

CU

ZI
X X X X

3
I
-d

h r l r l r l r l 0 0 0 0 rlrlrl,
rlrlrlrl 0 0 0 0 rlrlrlrl X X X X
-I=

0 3 r l C U O r l

CU

0
II

r l o

0 P - c o n
r
rlrlrlrl
% l X X X X
0r l 0 u 0 s '0 l c r rlrlrlrl

??-'.?

?0 Y0 o0 -30 ,

i h r l r l r l r l
-= I

l n \ O 3 3

c u 3 C U r l

. d

4 4 0 P-QQ ,,,A
I1
I- \

. d -I=

b-

rlrlrlrl X X X X

d -'o -'o -'o o

rlrlrlrl X X X X

k
M

0 C U 3 0 0 0 0 0

rlrlrlrl
X X X X

0 rl

r l O C U

0 0 0 0 r l r l r l r l

2 1

n \ O \ O

0 3 3

d o
rl X X
" 0

" -'o
rl X

-la " " " 0 0 0 r l r l d r l

X X X X

0 0 0 " r l r l

" 0 0 7 ' 0 0 0 0

CU,oco

. .
" C U \ O

" " r l r l X X X X

? t S ?
C-0

"

F9

"a,

rlk

Discussion

The c o n c e n t r a t i o n of r a d i o a c t i v i t y i n t h e coolant may be important t o t h e o p e r a t i o n and maintenance of t h e system because of t h e hazards of d i r e c t r a d i a t i o n from a nonleaking cooling system, o r of both d i r e c t r a d i a t i o n and i n h a l a t i o n of r a d i o a c t i v i t y from a l e a k i n g coolant system. The r e s u l t s of

t h i s study can be analyzed t o show t h e r e l a t i v e e f f e c t s on c o n c e n t r a t i o n s i n t h e coolant of 1) varying t h e r e s i s t a n c e t o d i f f u s i o n from t h e f u e l a s compared with 2) varying t h e r a t e of p u r i f i c a t i o n of t h e c o o l a n t . These

e f f e c t s can each be c o n t r o l l e d over wide ranges by design s p e c i f i c a t i o n s of t h e f u e l elements and t h e coolant system. The leakage r a t e f r o m t h e coolant

system can a l s o be c o n t r o l l e d by design, operations, and maintenance s p e c i f i c a t i o n s and a d m i n i s t r a t i o n . Thus, a balance can be made t o o b t a i n a n optimum combination of f u e l and coolant system designs, with t h e accuracy of t h e o p t i m i z a t i o n bounded only by t h e accuracy of t h e parameter d a t a . As a b a s i s f o r an i l l u s t r a t i v e p a r t i a l a n a l y s i s of t h e r e s u l t s , an o p e r a t i n g time of 1 0

8 sec

( 3 . 2 yr) was chosen t o i n c l u d e near-equilibrium

c o n c e n t r a t i o n s of t h e s h o r t e r h a l f - l i f e i s o t o p e s and s i g n i f i c a n t concentrat i o n s of t h e l o n g e r h a l f - l i f e m a t e r i a l s . A power of 100 Mwt was chosen

a s r e p r e s e n t a t i v e of t h e power range of many power r e a c t o r s and because t h e r e s u l t s a r e e a s i l y c o n v e r t i b l e t o o t h e r powers by a simple f a c t o r . 3 . and n u c l i d e s s e l e c t e d f o r comparisons. I n h a l a t i o n Exposures For each i s o t o p e t h e p o t e n t i a l i n h a l a t i o n dose was c a l c u l a t e d f o r f o u r v a l u e s of r a t each of two values of D ' f o r both cases I and 111. The a r e s u l t s a r e presented i n Table 2. Mathematically t h e c a l c u l a t i o n i s : Tables

5 p r e s e n t p o t e n t i a l a c t i v i t i e s i n t h e coolant of 1 2 r e p r e s e n t a t i v e

with these definitions:

TID P

=
= =

t o t a l i n t e g r a t e d dl3se f o r i n h a l a t i o n of - t h e coolant, rem. all power generated by - t h e f u e l elements combined all t o t a l number atoms i n t h e coolant gas, a t o m s / ( f i s s / s e c ) 1 f r a c t i o n decaying per second, sec f a c t o r t o convert pNgh t o pc x
v

Ng
A

=
=

F D

lom3, p c / ( d i s / s e c ) .

Value of

F
=

1/3.7 x 10' 10 mrem/pc

B u r n e t t ' s dose parameter,

The values of N g were obtained from t h e d i g i t a l computer r e s u l t s . Values of D* were obtained by r e c a l c u l a t i n g B u r n e t t ' s
Di
=

1957 values1'

of

73,800 F E . (RBE) FiT/:mi with t h e new values of t h e components a,i 1 reported i n 1959 by ICRP Commit'tee 11. The equation f o r t h e p o t e n t i a l dose a t a r e a c t o r power of 100 M w t

with t h e above d e f i n i t i o n s i s ;

TID

1 0 8.38 x 1 0
i

N~

= rem/(100 ~ w t )a t 10 s e c 8

To o b t a i n t h e TID t o a person, t h e TID t a b u l a t e d i s m u l t i p l i e d by t h e r a t i o of t h e r e a c t o r power t o >30 M w t times t h e f r a c t i o n of a l l t h e coolant gas which t h e person b r e a t h e s ( , t o t a l coolant gas breathed per t o t a l coolant

D i r e c t Radiation For each i s o t o p e t h e t o t a l gamma a c t i v i t y was c a l c u l a t e d f o r f o u r values of r a t each of two values of Da' f o r Cases I and 111. The r e s u l t s a r e presented i n Table

5.

Mathematically t h e c a l c u l a t i o n i s :

with t h e s e d e f i n i t i o n s :
A
=

gamna a c t i v i t y i n a l l t h e coolant gas, ( ~ e v / s e c ) / 1 0 0Mwt

*A

dose f a c t o r , not a d i f f u s i o n parameter.

p Ng
h

= = = = =

f i s s i o n power i n l e a k i n g f u e l elements, M w t t o t a l number atoms i n gas per f i s s i o n per second, atoms/fission-sec decay constant, d i s atom
-I

sec

E
F

mean t o t a l gamma energy per d i s i n t e g r a t i o n , Mev d i s f a c t o r t o convert t o ( ~ e v / s e c )per 100 M w t , F (fiss/sec)/100 Mwt
=

18 3.1 x 1 0 ,

The values of Ng were obtained from t h e d i g i t a l computer r e s u l t s . The equation f o r t o t a l ganrma a c t i v i t y i n all t h e gas with all f u e l elements leaking i s :

18 3.1 x 1 0

Nig

hi E

Mev s e c - ' ~ 0 0 Mwt) a t 1 0

8 sec

The r e s u l t would be m u l t i p l i e d by t h e r a t i o of t h e r e a c t o r power t o 100 Mw. Since d i r e c t r a d i a t i o n dose c a l c u l a t i o n s depend c r i t i c a l l y on t h e geometry of t h e coolant system and on t h e s h i e l d i n g e f f e c t s of components and s h i e l d s , no general statement on making these c a l c u l a t i o n s i s f e a s i b l e here.

E f f e c t of Removal Rate on Concentration i n Gas

It may be seen from Tablks 3 , and 5

i n c r e a s e i n r by a f a c t o r of 10 a t D' range of values of r from r e l a t i o n does not hold a s well. to

t h a t Ng (and t h e r e f o r e t h e concen-

t r a t i o n ) of rnost of t h e i s o t o p e s i s reduced by about a f a c t o r of 1 0 f o r each

=

to

Dl

10

-14

i n the

lom2.

A t smaller values of r, t h i s

Since t h i s a n a l y s i s does not s e p a r a t e t h e

e f f e c t s of leakage, p u r i f i c a t i o n , and deposition i n t h e removal of i s o t o p e s from t h e coolant, no conclusions can be drawn a s t o t h e i r r e l a t i v e e f f e c t s . Large values of p u r i f i c a t i o n removal of many of t h e i s o t o p e s could be obtained by passing all o r a l a r g e f r a c t i o n of t h e coolant through f i l t e r s , absorbers, o r chemical r e a c t a n t s . The f e a s i b i l i t y of each such operation,

and t h e f r a c t i o n of t h e flow t o be continuously t r e a t e d , would be s u b j e c t s f o r study and optimization i n each case. For example, pressure drop power

l o s s e s and maintenance and replacement c o s t s would have t o be considered.

E f f e c t of

Dl

on Concentration i n Gas

The q u a n t i t a t i v e e f f e c t of a given change i n D' on concentration i s l e s s p r e d i c t a b l e than f o r t h e same change i n r . i n t h e range r = -12 t o D1 Dl = 10 of D

-6 10
=

However, f o r most of t h e i s o t o p e s going from

to

t h e f a c t o r of decrease i n Ng i n
i s about 10, o r about a f a c t o r of
= 10-

-14 10

For t h e same range of r values i n going from D '

'

3 p e r decade
to D
=

lo-',

t h e f a c t o r of decrease v a r i e s more b u t i s i n t h e approximate range of

1 . 7 t o 2 per decade of D ' .

It would be expected t h a t t h e value of D t can be lowered considerably by
c o a t i n g t h e f u e l p a r t i c l e s , by obtaining uniform f u e l p a r t i c l e s of optimum. volume t o s u r f a c e a r e a r a t i o s , by c o n t r o l l i n g s i g n i f i c a n t i m p u r i t i e s i n t h e f u e l p a r t i c l e s , o r by i n c r e a s i n g t h e d e n s i t y of t h e p a r t i c l e s . progress has been made along each of t h e s e l i n e s f o r UO Some and

p a r t i c l e fuels,' 2 t h e r e i s no apparent reason why improvement i n o t h e r f u e l s would not be feasible

.
Dl

Some Considerations i n D 1 vs N g Relations Obviously, lowering t h e value of c e n t r a t i o n i n t h e gas. f o r an i s o t o p e w i l l lower i t s conHowever, t h e parent of an i s o t o p e with a low D 1 may I n such a case t h e concentration of t h e

have a comparatively high D ' .

daughter i n t h e gas, w i l l be l e s s dependent on t h e concentration of t h e daughter i n t h e f u e l , s i n c e a l a r g e r f r a c t i o n of t h e daughter i n t h e gas

w i l l have appeared from decay of t n e already-escaped parent.

The l a r g e r t h e

r a t i o of D 1 parent t o D ' daughter, t h e more pronounced t h i s e f f e c t w i l l be. Likewise, of course, t h e l a r g e r t h e r a t i o of h daughter t o h parent, t h e more pronounced t h i s same e f f e c t w i l l b e . A example of combinations of A and n
Dl

values f o r parent and daughter isotopes i n t h i s r e p o r t shows t h e tendency j u s t described, e s p e c i a l l y a t low values of time operated. From t h e computer output, t h e value of Ng (atoms fission-' sec'') for 1 ~ b " i s e s s e n t i a l l y constant a t 2.01 x 1 0 a f t e r l o 5 s e c o p e r a t i n g time with 1 D t = lo-' s e c The N~ of i t s daughter 5r90 i n c r e a s e s markedly with time

through a t l e a s t 1 0

8 sec

o p e r a t i n g time with D'

lo-',

a s would be The Ng of

. expected ( ~ i ~ 5s - 1 2 ) because of i t s l o n g (28-yr) h a l f - l i f e .

sQO

c o n s i s t s of two p a r t s , 1) t h a t r e s u l t i n g from decay of Rb90 which had The p a r t of t h e Ng of S r90

d i f f u s e d i n t o t h e gas before decaying and 2) t h a t which was formed i n t h e f u e l and subsequently d i f f u s e d out i n t o t h e gas.

r e s u l t i n g from decay of RbgO i n t h e gas may be c a l c u l a t e d a s follows:

where

S,d
=

atoms sr90 i n gas from decay of Rb90 i n g a s / f i s s / s e c

NRg

atoms RbgO i n gas ( c o n s t a n t ) / f i s s / s e c

time a f t e r r e a c t o r s t a r t u p , s e c

" s)%

decay constants of s r 9 0 and RbgO r e s p e c t i v e l y , s e c

The s o l u t i o n t o t h i s equation i s :

S d b s t i t u t i n g values of t = 1 05
N S, d

, 106, 1 07, and

6

1 08 s e c gives values of

a s follows :

t ( sec)

105

1 0

lo7

10

The d i f f e r e n c e between t h e s e values and t h e t o t a l values of Ng f o r s r 9 0 i n t h e gas taken from t h e t a b l e s r e p r e s e n t s t h e amount of s r 9 0 ( p e r f i s s i o n per second) which had d i f f u s e d d i r e c t l y out of t h e f u e l and had not y e t decayed, a s shown i n Table

6.

Table

6. Amounts of srgo i n Gas from

RbgO Decay and

srgODiffusion
t = 1 06 sec t = 1 07 sec

Source Term, & Condition Case (calculated

t = 1 05 s e c

= 10

8 sec

N~,d

8.48 x 10

8.48~10

8.48~10

8 . 1 3 ~ 140

above; D g

= lo-'')
9-50 x 1 0 1.62 x

2) NSg ( c a l c u l a t e d by 704,

lo3

7.90 x 1 0

3 . 6 9 ~ 160

Di
DI

=D6

=10-7)

3) NSg ( c a l c u l a t e d by 704,
a
=

8.65 x 1 01

9.27 x 10

1 . 6 1 ~ 140

7.55 x 1 05
r#

10-7, D ;
N

10-9)

4) N~~
Case

S, d

[case 2

0 8.2 x 1 0

2 7.72 x 1 0

7.05 x 1 0

3 . 6 1 ~ 16 0

11
= D ;
= 10

D ;

-7
1 . 7 x 10
0

5) N , ~ - N
Case

S,d

[case J

7.9 x 1 01

7.62 x 10

6 . 7 4 ~ 15 0

11

It can be seen t h a t , a t any time, decreasing

Dl

for

RbgO, Case J vs Case 2 above, s i g n i f i c a n t l y reduces t h e

srgOr e l a t i v e t o amount of srgO which

Dl

for had

diffused d i r e c t l y i n t o t h e gas and had not decayed. Table 6, Case 4 had t h e same D' f o r RbgO a n d s r g O , while Case 5 h a d D 1 f o r S r90 = 10-2 time D l f o r RbgO, and a t 10

sec a f t e r s t a r t u p , t h e amount of S r i n Case

4 i s more than f i v e times t h a t of

Case

5.
It i s a l s o of i n t e r e s t t o compare t h e amount of S r t h a t had d i f f u s e d as S r
= Di =

from t h e f u e l t o t h e t o t a l amount of S r i n the gas f o r t h e two cases D ' and D;

=

lo-'

D<

= 10".

A t s h o r t times (105 ) t h e r a t i o i s 0.0872

"8 2 f o r 93

D l - D b

and 0.0194

(s)

f o r t h e second case:

a t longer times

6.74 8 r e s p e c t i v e l y . It i s (10 ) t h e ratios a r e 0.978 ( 3*61) and 0.893 (-) 3.69 7.55 important t o note t h a t Dd may be a much smaller f r a c t i o n of D' t h a n a -1 was assumed f o r Case I1 o r Case I11 (10 and r e s p e c t i v e l y ) , i n which case t h e d i f f u s i o n .and decay of t h e parent may e s s e n t i a l l y determine t h e
N~ of t h e daughter.

It i s t h e r e f o r e important t o determine t h e values of

Of course, i f

D' of parent and daughter i s o t o p e s r e l a t i v e t o each o t h e r . p u r i f i c a t i o n and leakage r a t e s can be s p e c i f i e d accordingly.

t h e absolute D' values can be determined, t h e r e l a t i v e values follow, and

Conclusions and Recommendations Every f u e l considered f o r use i n a r e a c t o r should be s t u d i e d a s t o both t h e absolute and r e l a t i v e magnitudes of t h e d i f f u s i o n escape r a t e s of t h e fission-product elements from t h e f u e l , a s well a s t o t h e removal r a t e s from t h e coolant gas. While it i s evident t h a t i n c r e a s i n g t h e removal r a t e s from t h e gas can e f f e c t l a r g e reductions i n concentrations, it i s a l s o apparent t h a t reductions i n d i f f u s i o n r a t e s from t h e f u e l can produce s i g n i f i c a n t reductions of concentrations i n t h e gas. The s e v e r a l ways known f o r reducing t h e r a t e s of removal from t h e f u e l t o t h e coolant include 1) jacketing t h e f u e l elements a s with metal jackets, 2 ) coating t h e f u e l element with a d i f f u s i o n - r e s i s t a n t m a t e r i a l (such a s p r y o l y t i c graphite on graphite-based elements), 3) c o n t r o l l i n g t h e s i z e and shape of t h e f u e l p a r t i c l e s , and

4) i n c o r p o r a t i n g t h e f u e l
An a p p r o p r i a t e

p a r t i c l e s i n a d i f f u s i o n - r e s i s t a n t matrix such a s a metal.

balance between c o n t r o l of t h e d i f f u s i o n from t h e f u e l and removal from t h e gas i s f i n a l l y a c o s t engineering problem and may be expected t o be d i f f e r e n t f o r each type of f u e l element, coolant system, and d i f f e r e n t combinations of t h e two. Data a r e being developed on t h e D 1 values1 obtainable by f u e l treatment and manufacturing methods, and on r values a t t a i n a b l e by physical and chemical p u r i f i c a t i o n of t h e gas coolant. By t a b u l a t i n g and analyzing t h e p e r t i n e n t d a t a from t h e c a l c u l a t i o n h e r e i n f o r t h e ranges of D' and r of i n t e r e s t , an approximate optimum combination of design s p e c i f i c a t i o n s can t h e n be reached on a c o s t b a s i s t o a r r i v e a t required maximum s p e c i f i c a t i o n s of i s o t o p e concent r a t i o n s i n t h e coolant gas. I n a d d i t i o n , maximum leakage r a t e s from t h e

coolant system can be s p e c i f i e d t o f i t t h e maximum concentrations allowed i n t h e coolant i n a r r i v i n g at c o s t s of p r o t e c t i o n a g a i n s t damage from i n h a l i n g f i s s i o n products l e a k i n g from t h e coolant system. The magnitudes of t h e e f f e c t s on hazard p o t e n t i a l s of c o n t r o l l i n g t h e r a t e of escape from t h e f u e l and of p u r i f i c a t i o n of t h e coolant show t h e importance of determining fission-product d i f f u s i o n r a t e s i n f u e l s and coolant p u r i f i c a t i o n r a t e s , both a s functions of c o s t s , so t h a t optimum designs can be approached. Information i s needed on deposition r a t e s of f i s s i o n products from t h e coolant, both a s t o amounts deposited, r a t e s of deposition, and l o c a t i o n of concentrated d e p o s i t s . Such information would be valuable i n determining t h e s h i e l d i n g requirements a t all p a r t s of t h e system, t h e requirements f o r maintenance, and t h e minimum p u r i f i c a t i o n requirements.

I t appears t h a t t h e

complexity of t h e problem w i l l probably prevent a c c u r a t e t h e o r e t i c a l a n a l y s i s , and t h a t , t h e r e f o r e , most of t h e information needed must be determined experimentally. This study assumes values of t h e parameters D' and r and presents t h e r e s u l t i n g f i s s i o n product concentrations i n t h e coolant. include those of a c t u a l r e a l systems.

It does not analyze

any r e a l system except t h a t t h e range of values of D' and r a r e expected t o Furthermore, t h e r e s u l t s show some r e l a t i v e r e l a t i o n s between t h e e f f e c t s of changes i n t h e two parameters, and presents absolute values of concentrations f o r use a s a c c u r a t e d a t a become a v a i l a b l e on t h e removal r a t e s .

Appendix A . Nuclear P r o p e r t i e s of F i s s i o n Product I s o t o p e s Chain Atomic Mass and Branch

Chain Member

Nuclide

(sec'l)

toms

Fiss-l)

Fraction of Y

Appendix A . ( o o n ' t )

Appendix

4.

(wn't)

Appendix A. (con ' t )

N d '

F'm

Sm
N ' d

Appendix B Arrangement and Use of t h e IBM 704 Print-Out Tables Input Data The input d a t a t o t h e IBM 704 computer a r e shown i n Appendix A of t h i s report. These input d a t a used i n t h e c a l c u l a t i o n s were a b s t r a c t e d from of nuclide parameters. Appendix A i s a t a b u l a t i o n of 1)

Blomeke's tables1'

chain mass number, 2) nuclide code number ( f i r s t , second, t h i r d , o r f o u r t h member of t h e chain), 3) decay constant, A, of nuclide,

4) f i s s i o n y i e l d ,

y, of nuclide, and 5) f r a c t i o n , 6, of f i s s i o n y i e l d involved i n t h e decay chain branch i n d i c a t e d i n column 1.

It i s necessary i n many cases t o consult t h e input d a t a t o i n t e r p r e t

t h e IBM

mk

p r i n t - o u t of t h e c a l c u l a t e d r e s u l t s .

For example, t h e branches

of decay chains a r e c a l c u l a t e d a s separate chains, and t h e t o t a l concentrat i o n s of t h e nuclides a r e obtained by adding t h e r e s u l t s of t h e c a l c u l a t i o n s of t h e branches. For example, i n t h e mass-85 chain, t h e two branches a r e

added f o r 3.00 min barium, 4.36-hr krypton, and s t a b l e rubidium, but not f o r 85 1 2 10.27-yr krypton. (TO c l a r i f y , see t h e diagram of t h e decay chain of B r .) Thus, on t h e f i r s t page of t h e Case I i s o t o p e t a b l e , t h e t o t a l Ng f o r B r 85 1 1 i s o 0469377 x 10-I+ 0.117344 x 10-1 0.586 x 10-1 = atoms f i s s i o n sec a t T = 1 05 sec, D f =

0.521322 x

The t o t a l Ng f o r lib8> i s 0.244453 x 1 03 1 1 = 0.244 x 1 03 atoms f i s s i o n- s e c - . and r = 0 .

Computer Print-Out Table Headings The complete IBJI 704 p r i n t - o u t s of r e s u l t s a r e a v a i l a b l e although not included i n t h i s report. They organized i n t o t h e following t a b l e s : Each of t h e s e t a b l e s The values of Each i n d i v i d u a l isotopes, Cases I, 11, and I 1 r e s p e c t i v e l y . 1

i s divided i n t o subtables arranged i n order by parameter values. t h e parameters used a r e p r i n t e d a t t h e beginning of each subtable.

subtable has t h e p r i n t - o u t o r r e s u l t s arranged i n order by mass number. discussion of each t a b l e follows. Individual Isotopes, Case I . subtable values of
Dl,

A brief

A t t h e t o p of t h e f i r s t page of each
-I

r, and T ( d i f f u s i o n parameter, removal r a t e from gas,

and time a f t e r s t a r t u p ) a r e l i s t e d i n s e c - l , s e c

, and

sec respectively.

O n

each page t h e extreme right-hand column l i s t s f o r each row t h e chain mass number with an a d d i t i o n a l i n t e g e r t o i n d i c a t e t h e branch of t h e decay chain

f o r which t h e r e s u l t s a r e p r i n t e d i n t h a t row.

When t h e same nuclide

(isomer o r i s o t o p e ) appears i n two o r more separate rows, t h e t o t a l concentration i s obtained by adding t h e r e s u l t s , a s explained above. I n t h e Case I isotope t a b l e , t h e machine-printed values of D', r, and T a r e c o r r e c t and straightforward. Cases I1 and ----

I1 Isotope Tables.

The subtables f o r Cases I1 and I 1 1

isotopes a r e arranged i n t h e same order and with t h e same meanings a s t h e subtables f o r Case I isotopes, with t h e following exceptions :

1) To save computer time, only t h e mass chains 88 through 97 and

137 through 146 were c a l c u l a t e d f o r t h e s e two cases.

2)
i s D1 For t h e subtables headed T = a t h e D i n the heading i s D1 (DL = 0 . 1 DL b Case 111).

For t h e subtables headed T

0.1 x 10

( s e c ) , t h e D i n t h e heading
= 0.01

0 . 1 x 1 07, 0 . 1 x 1 08, and 0 . 1 x 109, f o r Case 1 ; D i 1

DL

for

Nuclide Sums, A l l Cases The t a b l e s f o r sums of nuclides f o r Case I a r e straightforward. To o b t a i n Case I1 nuclide sums f o r strontium, y t t r i u m , zirconium, niobium, barium, lanthanum, cesium, and promethium, t h e Case I1 t a b l e s of nuclide sums a r e used d i r e c t with D'
=

D) ;

= 0 . 1 DL

Results from sums

of o t h e r nuclides a r e obtained f r o m t h e Case I nuclide sums t a b l e s a s follows. For barium, krypton, rubidium, t i n , antimony, tellurium, iodine, xenon, and cesium, t h e r e s u l t s a r e obtained from t h e Case I sums t a b l e s with D ' For molybdenum, technetium, ruthenium, rhodium, neodymium, promethium, samarium, and europium, t h e r e s u l t s a r e obtained from t h e Case I nuclide sums t a b l e s with D '
=

= D ' a

0 . 1 DA

The D value l i s t e d a t t h e beginning of each

subtable i s D' b For t h e Case I 1 nuclide sums of strontium, yttrium, zirconium, niobium, 1 barium, lanthanum, cerium, and praseodymium, t h e Case I11 nuclide sums t a b l e s a r e used d i r e c t , with D '
=

Dd

For barium, kyypton, rubidium, t i n ,

antimony, tellurium, iodine, xenon, and cesium, t h e r e s u l t s a r e obtained from t h e Case I sums t a b l e s with D'
= Di

For molybedenum, technetium,

ruthenium, rhodium, neodymium, promethium, samarium, and europium, t h e r e s u l t s a r e obtained f r o m t h e Case I sums t a b l e s with l i s t e d a t t h e beginning of each subtable i s D ;

D1

0.01

D l

The D value

For i l l u s t r a t i o n , Table

7 l i s t s some examples.

Table

7.

I l l u s t r a t i o n s of Use of Sums Tables f o r Cases I1 and I11

Case -

Element

Find Concentration under Sums Table f o r D Case -

I
I

1 0-8 10- 1 1

I1 I11

1 0-lo

I
I 1 1

I1

1 0-13

APPENDIX C Arrangement and Use of Proposed Tables of Computer Output

It i s proposed t h a t t h e o r i g i n a l p r i n t - o u t t a b l e s from t h e IBM 704

computer be copied i n a more convenient arrangement and form f o r use f o r i n c l u s i o n a s an addendum t o t h i s r e p o r t a t some l a t e r d a t e . arranged t a b l e s . S e v e r a l complications i n t h e o r i g i n a l form, explained i n Appendix B, would be avoided i n t h e r e Table 8 i s a sample page of t h e proposed new format. The s i x t a b l e s There would be s i x t a b l e s of r e s u l t s i n t h i s addendum.

would present t h e c a l c u l a t e d N~ (number of atoms per f i s s i o n per second) of i n d i v i d u a l i s o t o p e s and of i n d i v i d u a l elements i n t h e gas coolant a s a f u n c t i o n of time a f t e r r e a c t o r s t a r t u p f o r Cases I, 11, and 1 1 The 1 . arrangement would be such t h a t each page p r e s e n t s t h e N g values f o r one i s o t o p e , isomer, o r element i n t h e coolant f o r one case number, f o r a l l s i x values each of D' and r, c a l c u l a t e d a t each of f o u r values of time a f t e r s t a r t u p . each t a b l e t h e element would be taken i n o r d e r by mass number. t h e chain would precede t h e page f o r t h e lower branch. The number of atoms i n a l e a k i n g f u e l element can be obtained by calcul a t i n g t h e t o t a l number p e r f i s s i o n p e r second i n a nonleaking element and s u b t r a c t i n g from i t t h e number i n t h e gas and m u l t i p l y i n g t h e r e s u l t by t h e number of f t s s i o n s per second i n t h e element. In I n cases of

two isomers of t h e same isotope, t h e page of r e s u l t s f o r t h e upper branch of

Table 8.

Concentrations of Individual

I s o t o p e s in Gas

(case I)
-1 ~ i s s - ' sec

Total At
Isotope

Atoms in Gas,

Time, seconds a f t e r s t a r t u p

r (sec-l)

D~~ (sec-')

-6 9.08 x l o m 6 1 . 0 9 x 3.11 x 3.85 x 1 . 0 1 ~ 1 0 1.26~10:; 3.21 x l o v 7 4.04 x 1.02 x 1 : 0: 1.28 x 10 3 . 2 2 ~ 1 0 4.06x10-~

9.08 x 3.66 x 1.25~10 4.06 x 1.29 x 1 : 0; 4.11~10

- 4 2.44

Missing -4 9 . 5 2 ~ 1 0 ~ 3.49 x 1014 1.16 x 10 3.72~10'~

x 10'~ -

References
1) W. B. C o t t r e l l , e t a1

., Fission-Product

Release from UO

2 '

Om-2935,

September 13, 1960. 2) J. D. Eichenberg, e t al., E f f e c t s of I r r a d i a t i o n on Bulk U02, WAPD-183, Chapter 1 1 S e c t i o n F, October 1957. 1, 3) J. A. Lane, e t al., A Study of Problems Associated with Release of F i s s i o n Products from Ceramic Fuels i n Gas-Cooled Reactors, ORNL-2851, S e c t i o n

3, October 27, 1959.

4) C o t t r e l l , op. cit., Tables V, VI, VII, VIII, and XIV.
W. Parker,

5 ) G.

e t al., F i s s i o n Product Release from UOp by High

Temperature D i f f u s i o n and Melting i n Helium and A i r , ORNL CF-60-12-14, December 1960.

6) C o t t r e l l , op. c i t . , p. 30.

7) P. I. Conn, e t al., I s o t o p e Deposition Hazards i n Gas Cycle Reactors,

presented a t t h e Annual Meeting of American Nuclear Society, Gatlinburg, Tennessee, June

17, 1959.

8) C o t t r e l l , op. c i t ., Table XVII.

9) A. H. Booth, A Method of C a l c u l a t i n g F i s s i o n G a s D i f f u s i o n fromUO2 Fuel and I t s a p p l i c a t i o n t o t h e Xr2-f Loop Tests, CRDC-721, p. 7.

10) T. J. Burnett, Reactors, Hazard vs Power Level, Nuclear Science and Engineering, Vol 2, 382-93 (1957).

1 ) Report of Committee I1 of t h e I n t e r n a t i o n a l C o d s s i o n on Radiological 1 P r o t e c t i o n on Permissible Doses f o r I n t e r n a l Radiation, 1959, r e v i s i o n .

1 2 ) J . 0 . Blomeke and M. F. Todd, P a r t I, Vol. I, Uranium F i s s i o n Product Production a s a Function of Thermal Neutron Flux, I r r a d i a t i o n Time, and Decay Time, 1. Atomic Concentrations and Gross T o t a l s , Om-2127, p. 13-39, August

19, 1957.

-116UNCLASSIFIED

lo7
TIME (sec)

Fig. 1.

Buildup of Fission Products in Coolant;

~ r ' ~ Case 1 , D'= , r = 0 to I (sec-'1.

UNCLASSIFIED O R N L - L R - D W G 60619

lof
TIME (sec)

Fig. 2.

Buildup of Fission Products in Coolant; ~ r ' ? , Case 1 , D'=

lo-'*,

r = 0 to I (set-0.

UNCLASSIFIED

ro7
TIME (sec)

Fig. 3.

Buildup of Fission Products in Coolant;

~r*',

Case I

D'= 10 7, r = 0 to 1

(set').

-113UNCLASSIFIED O R N L - L R - D W G 60621

lo7
TIME (sec)

Fig. 4.

Buildup of Fission Products in Coolant;

s r e g , Case 1 , D'= IO-",

r = 0 to 1 ( s e c ' ).

UNCLASSIFIED ORNL-LR-DWG 6 0 6 2 2

ro7
TIME (sec)

Fig. 5. Buildup of Fission Products in Coolant;

srgo, c a s e I , D'= 1 0 - ~ ~ = 0 to I (sec-l). r

-01 UNCLASSIFIEO ORNL-LR-DWG 6 0 6 2 3

4' 0
TIME (sec)

Fig. 6 . Buildup of Fission Products in Coolant;

srgO, Case I, D ' =

lo-",

= 0 to i. (sec-'1.

to-

10' TIME (sec)

Fig.

7 . Buildup of Fission Products in Coolant;

~ r ~ ~ ~ C a s e I ~ 0 ' =r = o0 o 1 ( s e c - ' ) . , 1 t
-12

UNCLASSIFIED O R N L - L R - D W G 60625

to'

lo7
TIME (sec)

Fig. 8 . Buildup of Fission Products in Coolant;

srgO, case11, D;

=lo- ,

r = 0 t o 1 (sec-'1.

UNCLASSIFIED ORNL-LR-DWG 60626

1o7

TIME (sec)

Fig. 9 . Buildup of Fission Products in Coolant;

srgO,Case 11, DL

= t0-12,

, = 0 to I (Sec-' -

UNCLASSIFIED O R N L - L R - D W G 60627

ro7
TIME (sec)

Fig. 10. Buildup of Fission Products in Coolant; srgO, Case 111, 0 = : r = 0 to 1 ( s e c ' 1.

UNCLASSIFIED ORNL-LR-DWG 6 0 6 2 8

90'

TIME Isec)

Fig. 1 1 . Buildup of Fission Products in Coolant; s r g O , Case 111,

DL

r = 0 to 1 (set').

to'

lo7
T I M E (sec)

Fig. 12. Buildup of Fission Products in Coolant;

srgO,Case 111,

0 = 10-12, .= 0 to 1 (set"). ;

107
TIME (sec)

Fig. 13. Buildup of Fission Products in Coolant; -7 Y'~,CCIS~I,D'=IO ,r-=oto~(sec-').

to7
TIME (sec)

Fig. 14. Buildup of Fission Products in Coolant;

y g O , case I , D ' = 10-I2 , r = o to1 (set').

lo7
TIME (sec)

Fig. 15. Buildup of Fission Products in Coolant;

ri3',

Case I , D'=

to-?,

r = 0 to 1 (sec-'1.

lor
TIME (sec)

Fig. 16. Buildup of Fission Products in Coolant;

~~~l~ Case

I , D'= IO-'*.

r = 0 to i

(set-').

47 0
TIME (sec)

Fig. 17. Buildup of Fission Products in Coolant ;

~ Case I , ~ =, ~ 01

r = 0 to 1

(set-0.

UNCLASSIFIED O R N L - L R - D W G 60635

1 o7

TIME (sec)

Fig. 18. Buildup of Fission Products in Coolant;

I ' ~ c~ s ,e I , D / = I O - ' ~ , r = o 10 1 ( s ~ c - ' 1. a

4 07

TIME (sec)

Fig. 19. Buildup of Fission Products in Coolant; -7 I ' ~ C a,s e I , ~ ' = 1 0 , r = O t o l ( s e c l ) . ~

UNCLASSIFIED ORNL-LR-DWG 6 0 6 3 7

to'

107

TIME (sec)

Fig. 20. Buildup of Fission Products in Coolant;

I ' ~ c a s e I , D'= 10~ ,

'* ,

= 0 to I

(set-0.

UNCLASSIFIED

1o7

TIME (sec)

Fig. 21. Buildup of Fission Products in Coolant;

C S ' ~ * , Case I , D l =

r = 0 to 1 (sec-'1.

lo7
TIME (secl

Fig. 22. Buildup of Fission Products in Coolant; - 2 r = o to I ( s e c t ) . cs13* Case I. D 10

'=

UNCLASSIFIED ORNL-LR-DWG 6 0 6 4 0

47 0
TIME (sec)

Fig. 23. Buildup of Fission Products in Coolant;

~ a ' ~ ' Case I, D' = , r = 0 to 1 (sec-').

1o7

TINIE (sec)

Fig. 24. Buildup o f Fission Products in Coolant;

6ai40, Case I , D ' =
r = 0 to I

(set').

-,/o-UNCLASSIFIED

1 o7

TIME ( s e c i

Fig. 25. Buildup of Fission Products in Coolant; ~a'~', Case I, D'=

r = 0 to I (set').

UNCLASSIFIED ORNL-LR-DWG 6 0 6 4 3

10'

TIME (sec)

Fig. 26. Buildup of Fission Products in Coolant;

~ a ' ~ ' ,Case I, D'= 10- lo r = 0 t o 1 (set'), ,

Fig. 27. Buildup of Fission Products in Coolant; ~ a ' ~ ' ,case I, D - 1o - ' ~ ,r = O to 4 (sec-' ).

'-

UNCLASSIFIED

ORNL-LR-DWG 60645

Fig. 28. Buildup o f Fission Products in Coolant;

~ o Case ' 11, 0; = ~

lod7, r ~ 0 ~ =

t o f (sec-'1.

UNCLASSIFIED O R N L - L R - D W G 60646

10'

TIME (sec)

Fig. 29. Buildup of Fission Products in Coolant; La 140, Case 11. D; = 10 -I2
I- =

to I (sec ).

-1

UNCLASSIFIED ORNL-LR-DWG 6 0 6 4 7

(07 TIME (sec)

Fig. 30. Buildup of Fission Products in Coolant;

~a ' 4 0 , Case 111, 0,: = lo-?,
I

= 0 to I (sec

-1

1.

40'
TIME (set)

Fig. 31. Buildup of Fission Products in Coolant;

~ a Case' 111, ~ = ~ 0 - ' ~ , ~ r = 0 to D; 1

(sec'l.

UNCLASSIFIED O R N L - L R - D W G 60649

to'

lo7
TIME (sec)

Fig. 32. Buildup of Fission Products in Coolant;

Laf4',

Case 111, D:=

lo-",

r = O t o 1 (sec-'1.

lof
TIME (sec)

Fig. 33. Buildup of Fission Products in Coolant;

~ e C a s e' 1. 0~ =
/

W 71-, 0 ~ = ~

to I

(set').

UNCLASSIFIED ORNL- L R - DWG 60651

10'
TIME (secl

Fig. 34. Buildup of Fission Products in Coolant;

Ce
144

, Case I, D'= 10- l2 r = O to I (set'). ,

47 0
TIME (sec)

Fig. 35. Buildup of Fission Products in Coolant; ~ r, C a s e I , ~ D l = ~ '

I-=0

to1 ( s e c 1.

-1

lof

TIME (sec)

Fig. 36. Buildup of Fission Products in Coolant;

~ r ' Case~ I, D / = 1 ~ , 0
-12

,r

= 0 to 1

(set').

Internal Distribution

1. J . W . A l l e n 2 . S . E. Beall 3. M. Bender 4 . A . L . Boch 5. R . B . Briggs 6. W . E . Browning 7. J. H . Coobs 8-17. W . B. C o t t r e l l 18. J . H. DeVan 19. D . A . Douglas 20. R. M. Evans M. H Fontana 2 22. J . F o s t e r 23. A . P. Fraas 24. B. L . Greenstreet 25. W . R . Grimes 26. W . 0 . Harms 27. H . W . Hoffman 28. J . O . KOD 29. R. B. Korsmeyer 30. J. L Lucius 31. R . N. Lyon 32. H . G. MacPherson 33. W . D. Manly 34. H . C . McCurdy 35. A. J . Miller

36 37.
38

39 40. 41.
42.

43 44. 45. 46. 47. 48. 49

50

51
52.

53. 54. 55-56. 57 58. 59-60. 61-63. 64-66. 67.

F. H . Neil1 L. G. Overholser G. W . Parker P. P a t r i a r c a A . M. Perry C . A. Preskitt M. W . Rosenthal o T. H . R w G . Samuels H . W . Savage A. W . Savolainen J. L . S c o t t 0 . Sisman M. J. Skinner I . Spiewak E. Storto J. A . Swartout D. B. Trauger C . S . Walker G. D . Whitman C . E . Winters M. M. Yarosh Central Research Library Y-12 Document Reference S e c t i o n Laboratory Records Dept . Laboratory Records - Record Copy

External D i s t r i b u t i o n

68. W . L . Albrecht (TVA) 69. W . R . Cooper (TVA)

70.

71.
72-86.

87. 88-89.

H . N . Culver (TVA) L . H . Jackson (AEC) Division of Technical Information Extension Research and Development Division, O 0 R Reactor Division, O 0 R