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ia~:af R3sear ch

D9pai t mei i i of the N a v y

Co n t r a c t Nonr - 220( 28)

ION EXCHANGE KINETICS

A NONLINEAR DI FFUSI ON PROBLEM

F. t -i el f f eri ch and M. S. Plesset

Engi neer i ng Di vi s i on

C4LI FCj RN1A I b ~ 5 S l I Vb J ~ E Of JECHPNOLOG'at'

Pasadena, Cal i f or ni a

Repcirt NO. 85-7

Sspern ber 1957

Ap p r o v e d b y

M S, PIesset

Office of Naval Res ear ch

Depart ment of the Navy

Cont r act ~ o n r - 2 2 0 ( 2 8 )

ION EXCHANGE KINETICS

A Nonlinear Diffusion Pr obl em

F. Hel fferi ch and M. S, Pl es s et

Reproduction i n whole o r i n par t is permi t t ed f or any purpose of

the United St at es Government.

Engi neeri ng Division

Cal i forni a Institute of Technology

Pasadena, Cal i forni a

Repor t No. 85-7

Sept ember , 1957

Approved by

M, S. Pl es s et

ION EXCHANGE KINETICS

A Nonlinear Diffusion Probl em

by

F, Helfferich and M. S. Pl es s et

Summary

Ideal limiting laws a r e calculated for the kinetics of particle dif-

fusion controlled ion exchange processes involving ions s f different

mobilities between spheri cal ion exchanger beads of uniform size and

a well- s t i r r ed solution, The calculations a r e based on the nonlinear

Nernst -Pl anck equations of ionic motion, which take into account the

effect of the el ect r i c f or ces (diffusion potential) within the system.

Numeri cal r esul t s for counter ions of equal valence and s i x different

mobility rat i os a r e presented. They wer e obtained by use of a digital

computer. Thi s approach contains the well-known solution to the cor -

responding l i near problem a s a limiting case. An explicit empi ri cal

formul a approximating the numeri cal r esul t s is given.

1, Introduction

An ion e'xsrchange r es i n consi st s essent i al l y of a three-dimensional,

cross-l i nked network of hydrocarbon chains carryi ng fixed ionic groups,

the el ect ri c charge of which is compensated for by mobile ions of opposite

charge ("csuater ions"'), These counter ions axe f r ee to diffuse within

the r esi n network, Tn contact with an electrolyte solution the r esi n t akes

up solvent and some additional mobile ions (additional counter ions, and

l' co-ions" have the same charge sign a s the fixed ionic groups). In a n

ion exchange process the counter ion speci es present initially i s replaced

by another speci es,

We consider the ion exchange between spheri cal ion exchange resi n

beads of uniform size containing the counter ion speci es A and a well-

s t i r r ed solution containing the counter ion speci es B, During the process

ions A diffuse out of the bead and a r e repl aced by an equivalent amount of

ions B.

Id has been established that such processes a r e diffusion controlled:

the r at e determining mechanism i s the interdiffusion of the two speci es

A and B, ei t her within the r esi n part i cl es o r i n a Nernst diffusion layer

("film"] adherent to the particle surface, which is not affected by st i rri ng,

1

Limiting law8 for fi l m controlled exchange in i deal syst ems have been given

previously. i n this paper i deal limiting laws for particle controlled

processes a r e calculated. Part i cl e control is favored by concentrated solu-

tions, l arge di amet er and high degree of cross-linking of the beads, and

efficient st i rri ng.

3

The driving ' tforce" for the flux of a n ionic speci es i s, i n systems

without convection, the gradient of i t s general chemi cal potential, the

principal el ement s of which a r e the concentration gradient of the speci es

and the gradient of the el ect ri c potential. Even if no ext ernal el ect ri c

field is applied, a gradient of the el ect ri c potential will, a s a rule, be

built up by the diffusion process (diffusion potential). The corresponding

differential equations a r e nonlinear. The interdiffusion process con-

si dered here can be descri bed in t er ms of one interdiffusion coefficient

which, however, is not constant but changes with the concentration rat i o

of the two counter ion speci es present. Hence, the mathematical t r eat -

ment is that of a diffusion problem with varying diffusion coefficient,

Hitherto only the corresponding linear problem, i. e. , with constant i nt er-

4

diffusion coefficient, has been solved and applied to ion exchange

kine t i cs. In our approach the solution to the linear problem r epr e-

sent s a limiting case: the exchange of counter ions of equal mobility.

The linear solution holds rigorously for isotopic exchange processes,

whereas for ot her cas es the deviations a r e considerable,

2. Model and Simplifying Assumptions

We use the si mpl est model conceivable and the si mpl est equations

proven to be adequate for the description of ionic diffusion processes, the

Nernst -Pl anck equations.

11-15

Without respect to i t s act ual porous st ruct ure the whole r esi n is

t reat ed a s a quasi-homogeneous phase. Individual diffusion constants for

the mobile ions present a r e defined correspondingly; they can be measured

by t r acer techniques in equilibrium syst ems. 1' 15-18 The assumption is

niade with exper i ment al support 15' 16' l8 t hat t hese individual diffusion

const ant s ar e, essent i al l y constant f or a given r esi n, i, e. , independent

of ionic composition. We make use of the i deal Ei nst ei n r el at i on between

the individual diffusion const ant s and the el ect r ochemi cal mobi l i t i es, We

neglect any coupling of ionic fluxes ot her than by el ect r i c f ar ces. We

as s ume a const ant concent rat i on of fixed ionic groups throughout the r esi n.

Any concent rat i on change and flux of the co-i ons i s di sr egar ded, si nce

they a r e s mal l a s compar ed with those of the count er i ons i f the concen-

t r at i on of the solution i s not too high and that of the fixed ionic groups not

too low. l3 We negl ect changes in ionic act i vi t y coefficients and swelling

condition of the r e s i n a s wel l a s the effect of gr adi ent s aP swelling pr es -

s ur e . Under the si mpl e boundary condition used her e, the magnitude of

the sel ect i vi t y coefficient i s i r r el evant . l9 We r es t r i ct our s el ves to

r adi al diffusion, i. e . , spher i cal symmet r y. We as s ume that i nt erdi f-

fusi on within the r es i n beads i s the r at e det ermi ni ng mechani sm through-

out the pr ocess. Thi s l ast assumpt i on i s not st r i ct l y valid; i t l eads to

exchange fl uxes t hat a r e infinite initially, wher eas the possible diffusion

r at e through the f i l m is finite. F o r a ver y s hor t i ni t i al period f i l m

diffusion mus t be the r at e controlling step.

The assumpt i ons and simplification l i st ed above a r e those usually

made i n the formul at i on of a model f or i on exchange ki net i cs.

5- 10

We do not negl ect the effect of the el ect r i c potential gradi ent on the

ionic fl uxes; i n t hi s r es pect our appr oach di f f er s f r om previous t heori es.

3, Formulation of the Pr obl em

Under the assumpt i ons mentioned, the fluxes of the two counter ion

speci es A and B a r e given by the Nernst -Pl anck equations

11-14

O B = - D B r ad CB -I zBCB (F/./RT) grad rg] ,

I l b)

where @ is the flux, 2) i s the individual diffusion constant, G i s the

mol ar concentration, z i s the el ect rochemi cal valence, is the

Far aday constant, R is the gas constant, T i s the absolute t emperat ure,

i s the el ect r i c potential, and the subscri pt s A and B r ef er to the

counter ion speci es,

El ect roneut ral i t y requi res that the total equivalent concentration of

counter ions is constant throughout the bead, since the concentrations of

both the fixed ionic groups and the co-ions a r e constant; thus

The absence of an el ect ri c cur r ent in combination with (2) gives the con-

dition

By use of (2) and (31, Eqs. ( l a ) and ( l b) may be combined to give

2

D ~ D ~ ( ~ ~ ~ ~ + .BeB)

2

grad CA .

D A A A zZ c + DBz BCB

%

'She quantity in bracket s may be t ermed the interdiffusion coefficient

D~~

of the process, Its value depends not only on the individual dif-

fusion constants DA and Dg; it i s al so a function of the concentration

rat i o cA/cB and t herefore a function of the time and space coordinates.

The dependence of the interdiffusion coefficient on ionic composition i s

shown in Fi g. 1 for various values of the rat i o D~ / D* . For CA 6( CB9

DAB as s umes the value DA, and f or CB ( CA the value DB. The ion

present in smal l er concentration always has the st ronger influence on

the interdiffusion coefficient. 33 l9 Thi s simple rul e i s a consequence of

of the fact that in (1) the concentration of the speci es ent er s i n the el ec-

t r i c t erm. It is al so physically evident since the el ect r i c field act s on

ever y ion present and thus causes a l arge t ransference of the species

present in high concentration, whereas the flux of the speci es present in

low concentration is hardly affected.

For the t reat ment of time dependent processes the equation of con-

tinuity must be introduced

In previous work on time dependent processes, only the limiting

l i near case has been considered, to which (4) and (5) reduce when a

constant interdiffusion coefficient DAB is assumed. Analytical solutions

to the linear problem have been derived for a number of syst ems including

those with spheri cal symmet ry with vari ous boundary conditions.

4, 20

However, Eq. (4) and Fig. 1 show that the assumption of a constant i nt er-

diffusion coefficient holds only i f the individual diffusion constants DA and

D a r e equal, a s is the case for example i n isotopic exchange processes.

B

Thi s paper de a l s with the general, nonlinear problem and will t reat

s pe~i f i cal l y syst ems with spheri cal symmet ry. Upon substitution of (4)

into (5) an expressi on i s obtained which can be wri t t en conveniently i n

dimensionless f or m with the introduction of the following dimensionless

vari abl es and paramet ers:

a s z D / z D - 1 ;

A A B B

b = aA/zB - 1

where t is time, r is the radi al coordinate, and ro is the radi us of the

beads. The resul t i ng equation

was derived i n a prel i mi nary note. The fract i on qA of the speci es A

st i l l present i n the sphere a t the dimensionless t i me T is expressed i n

t e r ms of the solution y ( p, .c ) of Eq. (7) a s follows:

The ion exchange r at e, deiined as the decr ease with time of the amount

QA of the speci es A (in mol es) present i n the spheres, may be written a s

where V is the t ot al volume of ion exchanger used.

If the problem is limited to the exchange of counter ions of equal

valence (zA = zB)$ SO that b = 0. the general equation (7) may be

simplified by the iniroduction of the new variable

to be come

which is a convenient f or m for numeri cal integration. The r esul t s

report ed a t the present time will be f or this case. Determination of the

solutions of Eq, (7) for non-zero values of b a r e planned for a l at er time.

We use the simple s t initial and boundary conditions possible, assumi ng

that initially the beads contain counter ions A only and the solution counter

ions B only, and that no concentration changes occur i n the solution,

The boundary condition (12b) corresponds to infinite solution volume or

to continuous renewal of the solution, The selection of initial and bound-

a r y conditions ot her than (12) would requi re the introduction of furt her

par amet er s which, for the numeri cal evaluation we car r i ed out, would

have to be chosen ar bi t r ar i l y and have l ed to r esul t s applicable i n speci al

cas es only. In cont rast , by using the conditions (121, mor e general l i mi t -

ing laws a r e obtained, which can be approached fai rl y closely by experi-

ment al techniques.

Even under the simple conditions (12) a n analytical solution to the

Eqs. (7) o r (11) was not obtained,

We have evaluated (11) numerically for

si x values of the rat i o D ~ / D ~ of the individual diffusion constants:

The result; a r e given i n section (5).

4. Calculation Procedure

For the numeri cal evaluation, (11) was approximated by the finite

difference f or m

- R- ( P) [u(P, 7 - u(P-AP,.I)]

where

g(p, = exp - 4 ~ 3 T If A 7 / ( AP ) ~ ;

By use of (13), U(P, z + h 7 ) can be calculated f r om u( p+~p, T ),

u(pI 1~ ), and u ( p - 4 , T ).

For the calculation the initial condition and the

boundary conditions for p = 0 and p = ]I a r e requi red. The initial

condition is obtained f r om (12a) and (10):

\

The boundary conditions a t the bead surface ( P = 1) i s given by (12b) and

It can be shown that the gradi ent s of y and u vanish a t the center of the

sphere:

( a u / a P I P ' 0 = o .

Hence the condition a t p = 0 becomes

By choice of Ap an upper limit is given for A T by the stability

condition f or the numeri cal integration. 22 In case of (131, this condition

The function u(p, 7 ) was calculated numerically f r om (13) and (14)

i n accord with the requi rement (15).

For the numeri cal integration corresponding to (a), which leads to

the fract i on qA st i l l present in the sphere, Si mpsonf s rul e was used:

where

The di mensi onl ess r at e, -dqA/d r, was approxi mat ed by

The cal cuht i on s t ar t s out with a step' function, Therefore, a ver y

fine subdivision of space and t i me is r equi r ed initially, The i ni t i al

spacing of p used was Ap = l/640, The spacing of AT was

sel ect ed i n accor dance with the stability condition (15).

As the cal -

culation proceeded, Ap was i ncr eased stepwise to 1/320, 1/160,

1/80. 1/40 ( at about qA = 0. 9) , 1/20 ( at about qA = 0.6), and 1/10 (at

qA 4 0.1). AT was i ncr eased correspondingly. The est i mat ed max-

4-

irnurn e r r o r i n qA is t 0.01; the e r r o r i n dqA/d.r i s about - 2%.

The cal cul at i ons wer e car r i ed out on the "Datatronl' digital com-

puter (manufact ured by El ect rodat a, Inc. , Pasadena, California) in the

computing cent er a t the California Institute of Technology. Floating

point number s wer e used. The total t i me r equi r ed was about 35 hours.

5. Resul t s and Di scussi on

The calculation yi el ds the dimensionle s s functions u ( ~ , 7 ), qA( s ),

and -dqA( T ) / d l . The f i r s t i s readi l y convert ed to y (p. .r ), which

gi ves the r adi al concentration profiles of the speci es A. In tabulating

and plotting the r esul t s, we have followed gener al pract i ce and given

the f r act i onal at t ai nment of equilibrium, ~ ( s ), r at her than qA(7 ).

Under the i ni t i al and boundary conditions (121, t hi s quantity is given by

F ( 7 ) = 1 - qA( 7 ) (18)

The r epr esent at i on of the data i s kept i n di mensi onl ess f or m, since the

act ual values of the concentrations, the fract i onal attainment of equilib-

ri urn, and the r at es a t a given time t depend al so on D A# ro, C, and V.

They can be obtained frqm the tables and graphs by substituting numcri -

cal values for these quantities and using ( 6 ) and (9).

Table I gives the fract i onal attainment of equlibriurn,

F( T ), and

the dimensionless rat e, -dq / d q l for the vari ous cases. Fi gure 2

A

shows a plot of F ver s us T and includes the solution to the linear ease

4

(DA = DB) which is well known to be

2 2

cup(-n a T) . (19)

F ( T ) = f - -

mi! n = ~ n

It should be emphasized that the time coordinate T ~ont a i ns the

quantity DA; hence, these r esul t s can be used f or di r ect comparison of

different processes only i f the ion A initially present in the beads i s the

same in a l l cases. Fi gur e 2 shows that the curves for different rat i os

D ~ / D ~ can not be t ransformed into one another by a linear t ransforma-

tion of the time. If the ion B is s b we r , the process i s slower, but not

by a constant fact or, because the interdiffusion coefficient i ncr eases with

decreasi ng concentration of A, On the ot her hand, i f B i s f ast er , the

process i s fast er, but the interdiffusion coefficient decr eases during the

process.

It is of i nt er est to compare the r at es for forward and backward

exchange of two counter ion species. In Fi g, 3 we have plotted the f r ac-

-I-

tional attainment of equilibrium for the exchange processes H against

+ -I-

13' and Li agai nst H , assumi ng a rat i o D ~ / D ~ ~ = 10. For di rect

compari son we have chosen D t / r 2 a s the dimensionless time

H o

coordinate in both cases, i t is seen that the process is fast er i f H ' , the

f ast er ion, *i s initially present in the resi n, The half t i mes of exchange

differ by about the factpr 2, the time requi red f or 90% exchange by about

Che factor 3. According to previous t heoi i es, which assume a constant

interdiffusion coefficient, the two curves should coincide.

The radi al concentrakion profiles of the speci es A for 25%, 50%,

75%, and 90% exchange a r e shown in Fi g, 4. The profiles for the linear

case (D* = ~ g ) given by

4

2 2

sin (nnp) exp (-n n T ) (20)

T P , = 1 n

a r e included. The shape of the profiles depends strongly on the ratio

DA/Dg

If the ian present in the sphere initially is much the fast er one,

a comparatively sharp boundary moves i n toward the cent er of the bead

(I?ig. 4a). If the ion present in the bead initially is much the slower one,

the boundary is diffuse and the process reaches the center rapidly

(Fig. 4b). Again, the explanation is straightforward.

In the f i r st case

the concentration of the fast er ion is s mal l near the surface and large

near the cent er of the bead. Hence, the interdiffusion coefficient

decr eases toward the center.

Therefore the out er shells of the bead ar e

exhausted rapidly, whereas the exchange near the cent er remai ns slow,

In the second case, the opposite holds, The interdiffusion coefficient

i ncr eases toward the cant er; therefore the exhaustion is mor e uniform.

Previ ous t heori es lead to one set of curves for a l l cas es (Fig. 4g).

Fo r pract i cal purposes, an explicit expressi on for F ( .c ) which

approximafes the numeri cal r esul t s will be useful. The relation

~ ( 2 ) =

2

- exp Cn ( f l ( a ) e t f 2( a) z2 + f 3 ( a ) ' z. ~)J] 1/2

where a =: D ~ / D ~ and the coefficients f a), f2( a ) , and f 3( a ) a r e

given by

t

f i t s al l the numeri cal r esul t s within a n e r r o r of - 6%. It should hold

equally wel l f or i nt ermedi at e values of the rat i o D ~ / D ~ . Equation (21)

was developed a s an extension of a si mpl er but l e s s accurat e approxi-

mation given by vermeul enZ3 f or the linear case.

We wish to emphasize again that the r esul t s r epr esent i deal limiting

laws only, f r om which the behavior of act ual syst ems may be expected to

show mor e or l es s pronounced deviations. However, the comparison with

the solution f or the linear case demonst rat es conclusively that the effect

of the el ect r i c potential included i n our approach is an essent i al feat ure of

the process which no theory can omit.

4. Acknowledgments

We a r e indebted to Drs. J. Franklin, C. B. Ray, and R. Nathan

f ox helpful suggestions concerning the numeri cal integration. We al so

wish to expr es s our gratitude to Mr . D. Brouillette and Mi ss Z. Lindberg

f or t hei r valuable assi st ance i n the computations.

FRACTIONAL ATTAINMENT OF EQUILIBRIUM, ~( t ) , AND DIMEI\TSIONLESS

RIZTE, - aqA(*)/a+ , FOR SIX D ~ W I T VALUES OF THE RATIO D ~ / D ~

TABLE I ( ~ o n t ' d , )

FRACTIONAL ATTAJXMENT OF EQUILIBRIUM, F ( * ) , AND DIMEXVSIONLESS

RATE, - dqA( r ) i d s , FOR SIX DI FFERWT VALUES OF 'PHE RRTIO ~ ~ 1 %

TABLE I (~ont'd.)

%

FRACTIONAL ATTAUNMENT OF EQUILIBRIUM, F( * ) , AND DLMENSIOIEZSS

RATE, - dqA( ( )/ d z , FOR SIX D~~ VALUES OF THE RATIO ~ ~ 1 %

TABLE I (C!ontfd,)

1

FRACTIONAL ATTAINMENT OF EQUILIBRIUM, F( ) , AND DIMENSIONLESS

RATE, - dqA( l ) / d~ FOR SIX DIFFEBEXQ VALUES OF THE RATIO D ~ / D ~

a) ~ ~ 1 % - 1/2

TABLE I (cont9d. )

x

FRACTIONAL ATTAINMENT OF EQUILIBRIUM, F( Z ) , AND DIMENSIONLESS

UTE, -aql((% ) / a~ , FOR SM ~rn- VALUES OF TIE WTO D ~ / D ~

FRACTIONAL ATTAIJSTMENT OF EQUILIBRIUM, F(*E' ), AND DLMENSIONLESS

RATE, - aqA(-z )/

, FOR SIX DIFFERENT VALUES OF THE RATIO D ~ / D ~

EQUIVALENT FRACTION OF B EQUIVALENT FRACTION OF B

Fig. 1. Dependence of the interdiffusion coefficient DAB on the ionic

composition of the exchanger, calculated from Eq. (4), for

the interdiffusion of ions of equal valence (left) and of a uni-

valent and a bivalent ion (right). The different curves cor-

respond to different ratios D* / D~ .

CH- pA

O 0.2

u .4 u

$"1&

b""; V

.*-+ 2

2% 2 ,

ZJ+\

4 +h X

IT.; <

0)

2 ; f.9;

U &I-*

*v c d *

k+?* e - c W

CrXJ d.2

1

( a) DA / DB=I O

W

-I

a

(el DA/DB= 2

> - 1.0

3

0

W

0.5

0

0 0. 5 1.0 0 0. 5 1.0

RADI AL COORDINATE p

'

RADIAL COORDINATE p

RADIAL COORDINATE p

Fi g. 4. Concentration profiles of the speci es A i n the bead for 2570,

5070, 7570, and 90% exchange (F = 0 . 2 5 , 0 . 5 0 , 0 . 7 5 , and 0. 90)

for seven different rat i os DA/ DB. The profiles for t he linear

case (DA = DB) wer e calculated f r om Eq. ( 20) .

<

Ref er ences

1

4;. E. Boyd, A, W. Adamson and L, S. Myer s. , Jr. , J. Ame r ,

Chem. Soc. , Vol. 69, p. 2836, 1947.

$1

R. Schlogl and F, Helfferich, J. Chem. Phys. , Yol. 26, p. 5, 1957,

F, Hel fferi ch, Angewandte Chem. , Vol 68, p 693, 1956

R. M. Ba r r e r , "Diffusion i n and through sol i ds, " Cambri dge

Pr e s s , 1941, p. 29.

D. E. Conway, J. H. S. Gr een and D. Reichenberg, Tr ans .

Fa r a da y Soc. , Vol 50, p. 51 1, 1954.

D. K. Hal e and 19. Rei chenberg, Disc. Far aday Soc., Vol. 7,

p. 79, 1949.

T. R. E, Kr es s man and J. A. Ki t chener, Di sc, Far aday Soc, ,

Vol. 7, p. 90, 1949.

J. B. Rosen, J, Chem. Phys. , Vol. 20, p 387, 1952.

D. Rei chenberg, J. Amer . Chem. Soc. , Vol. 75, p 589, 1953.

E. Glueckauf, Tr ans . Fa r a da y Soc. , Vol. 51, p 1540, 1955.

W. Ner nst , Z. Phys. Chem. , Vol. 2, p. 613, 1888; Vol. 4,

p. 129, 1889.

M. Pl anck, Ann. Phys. u. Chem. , Vol. 39, p 161, 1890.

T. Teor el l , Z. El ekt r ochem. , Vol. 55, p. 460, 1951.

R. Schdgl , Z. Phys. Chem. , N. F. , Val. 1, p. 305, 1954.

F. Hel fferi ch und H. D. Ocker , Z. Phys. Chem. , N. F.

Vol. 10, 213, 1957.

B. A. Soldano and G. E. Boyd, J. Amer . Cliem. Soc. ,

Vol. 75, p. 6107, 1953.

M, Tetenbaurn and H. P. Gr egor , J. Phys, Chem. , Vol. 58,

p. 1156, 1954.

B. Stein, Thesi s, ~ G t t i n ~ e n , 1957.

F. Hel fferi ch, Disc. Far aday Soc., Vol. 21, p. 83, 1956.

S. Pat t er son, Pr oc. Phys. Soc. o on don), Vol. 59, p. 50, 1947.

F. Hel fferi ch and M. S. Pl es s et , J. Chi mi e Physique, i n pr ess.

R. Courant , K. Fr e dr i c hs and N. Lewy, Mat hemat i sche Annalen,

Vol. 100, p. 32, 1928.

T. Vermeul en, Ind. Engng. Chem. , Vol. 45, FA 1664, 1953.

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Navy 100, Fl e e t Po s t Offi ce

New Yor k, New Yor k (25)

Chi ef, Bur e a u of Or dnance

Navy Depar t ment

Washi ngt on 25, D. C.

At t n: As s t , Chi ef f or Re s e a r c h

(Code Re)

Sys t cr ns Di r ect or , Under -

( 1)

wa t e r Or d (Code Rexc)

Ar mor , 130nlb, Pr oj ect i l e,

(1)

Rocket , Gui ded Mi s s i l e Wa r -

head and Bal l i s t i cs Br anch

(Code Re3) ( 1 1

Tor pedo Br anch ( code Re6) (1)

Re s e a r c h and Component s

Sect i on (Code Reba)

Mi ne Br anch (Code Re7)

( 1)

( 1)

Chi ef, Bur e a u of Shi ps

Navy Depar t ment

Washirigton 25, D. C.

Attn: Re s e a r c h and Devel op-

ment (Code 300)

Shi p Desi gn (Code 410)

( 1 1

Pr e l i mi n a r y Desi gn and

( 1)

Shi p Pr ot ect i on (Code 420) (1)

Sci ent i fi c, St r uct ur al and

Hydr odynami cs (Code 442) ( 1)

Submar i ne s (Code 5 25)

Pr o p e l l e r s and Shaft i ng

( 1)

(Code 554) ( 1)

Di r ect or Chi ef, Bur e a u of Yar ds and

Naval Re s e a r c h La bor a t or y Docks, Navy Depar t ment

Washi ngt on 25, D. C, Washi ngt on 25, D. C.

At t n: Code 2021 ( 6 ) Attn: Re s e a r c h Di vi si on ( 1)

Chi ef, Bur eau of Aer onaut i cs

Navy Depar trnent

Washi ngt on 25, D. C.

At t n: Re s e a r c h Di vi si on

Ae r o and Hydr o Br a nc h

( Code Ad-3)

Appl . Mech. Br a nc h

( Code DE-3)

Commander

Naval Or dnance Te s t St at i on

3202 E, Foot hi l l Bl vd.

( 1) Fks adena, Cal i f or ni a

At t n: Hcad, Under wat er Or d. ( 1)

(1) Head, Re s e a r c h Div. ( 1)

(1) Commander

Naval Qr dnance Te s t St at i on

Inyokern, Chi na La ke , Cal i f.

At t n: Techni cal Li b r a r y (1

Commanding Officer and Di r ect or

David Tayl or Model Basi n

Washington 7, D. C.

Attn: Hydromechani cs Lab.

Seawo r thine s s and Fl ui d

(1)

Dynami cs Div.

Li br a r y

Commanding Officer

Naval Ordnance Labor at or y

White Oak, Maryland

Attn: Underwater Or d. Dept. (1)

Commanding Officer

Naval Underwater Ordnance Sta.

Newport, Rhode Isl and (1)

Di r ect or

Underwater Sound Labor at or y

Fo r t Trumbul l

New London, Connecticut (1)

Li br ar i an

U. S. Naval Post gr aduat e School

Monterey, California (1)

Executive Secr et ar y

Res ear ch and Development Boar d

Depart ment sf Defense

The Pentagon

Washington 25, D. C. (1)

Chai rman

Under seas War f ar e Commi t t ee

National R e s ear ch Council

210 1 Constitution Avenue

Washington 25, D. 6 , (1)

Dr. J. El. McMillen

National Science Foundation

1520 I4 St r eet , N. W.

Washington, D. C. ( 1)

Di r ect or

National Bur eau of St andar ds

Washington 25, D. C.

-4ttn: Fl ui d Mecha.nic s Section

( I )

Dr . G, H. Keulegan

National Hydraulic Labor at or y

National Bur eau of St andar ds

Washington 25, D. C. (1)

Di rect or of Resear ch

National Advisory Commi t t ee

f or Aeronaut i cs

1512 H St r eet , N. W.

Washington 25, I). C. 0)

Di r ect or

Langley Aeronautical Labor at or y

National Advisory Commi t t ee

f or Aeronaut i cs

Langley Fi el d, Virginia (1)

Mr . J. B. Par ki nson

Langl ey Aeronaut i cal Labor at or y

National Advi ssry Commi t t ee

f or Aeronaut i cs

Langley Fi el d, Virginia ( 1)

Commander

Ai r Re s ear ch and Development

Command

P. O. Box 1395

Bal t i more 18, Maryl and

Attn: Fl ui d Mechani cs Div. ( I )

Di rect or

Waterways Exper i ment Station

Box 631

Vicksburg, Mi ssi s sippi (1)

Beach Er osi on Boar d

U. S . Ar my Cor ps of Engi neer s

Washington 25, D. G, (1)

Office of Ordnance Res ear ch

Depart ment of the Ar my

Washington 25, D. G. (1)

Office of the Chief of Engi neer s

Depart ment of the Ar my

Gravelly Point

Washington 25, D: C. (1)

Commi ssi oner

Bureau of Recl amat i on

Washington 25, D. C. (1)

Di rect or

Oak Ridge National Labor at or y

P. 0. Box P

Oak Ridge, Tennessee (1)

Di r ect or

Applied Physicsk Division

Sandia Labor at or y

Albuquerque, New Mexico (1)

P r o f c ~ s o r Ca r l E c k a r ~

Scr i pps 111s ti t ut e of Oceanogr aphy

L,a .Jolla, Cal i forni a

(1)

Do c u p e n t s s e r v i c e Cent er

A-i-med Ser vi ces Techni cal

I nf or mat i on Agency

Kno tt Bui l di ng

Dayt on 2, Ohi o (5)

Offl ce of Techni cal Se r vi c e s

Depar t ment of Comr ner ce

'Washington 2-5, D. C. (1)

Pol yt , echni c Inst i t ut e of Brookl yn

Depar t ment of Aer onaut i cal

Engi neer i ng and Appl i ed Mech.

99 Li vi ngst on St r e e t

Brookl yn I , New Yor k

At t n: Pr o f , H. Re i s s ne r (1)

Di vi si on of Appl i ed Mat hemat i cs

Br own Uni ver si t y

Pr ovi dence 12, Rhode I sl and (1)

Cal i f or ni a I nst i t ut e of Technol ogy

Pas adena 4, Cal i f or ni a

Attn: Hydr odynami cs La bor a t or y

Pr o f e s s o r A. Hol l ander

Pr o f e s s o r R. T. Knapp

Pr o f e s s o r M, S . Pl e s s e t

I

Pr o f e s s o r V. A, Vanoni

(1)

GALCIT

(1)

Pr o f , G. E3. Mi l l i kan, Di r ect or (1)

Pr of . Har ol d Wayl and (1)

Uni ver si t y of Cal i f or ni a

Ber kel ey 4, Cal i f or ni a

At t n: Pr o f e s s o r H. A. Ei ns t ei n

Dept , of Engi neer i ng

Pr o f e s s o r El, A, Schade,

(1)

Di r , of Engr , Re s e a r c h (1)

Ca s e I nst i t ut e of Technol ogy

Depar t rnent of Mechani cal Engi neer i ng

Cl evel and, Ohi o

At t n: Pr o f e s s o r G, Kuer t i 0)

Cor nel l Uni ver s i t y

Gr aduat e School af Aer onaut i cal

Engi neer i ng

I t haca, New Yor k

Attn: Pr o f , W. R* Se a r s , Di r ect or ( 1)

H a r w r d Uni ver si t y

Dept. of Mat herrl at i cs

Cambr i dge 38, Mas s .

At t n: Pr of . G. Birkhoff

Uni ver s i t y of Il l i noi s

Dept. of Theoret i cal . and

Appl i ed Mechani cs

Col l ege of Engi neer i ng

Ur bana, I l l i noi s

Attn: Dr , J. M, Rober t s on

Indi ana Uni ver s i t y

Dept. of Mat hemat i cs

Bl oomi ngt on, Indiana

Attn: Pr o f e s s o r D. Gi l bar g

St at e Uni ver s i t y of Iowa

Iowa Inst i t ut e of Hvdr aul i c

Re s e a r c h, Iowa Ci t y, Iowa

Attn: Dr . Hunt er Rouse, Di r

Uni ver s i t y of Mar yl and

I ns t . f or Fl ui d Dynami cs and

Appl i ed Mat hema t i cs

Col l ege Pa r k , Mar yl and

At t n: Pr of . M. H, Mar t i n,

Di r e c t or

Pr of . J. R. Weslce

Mas s achus et t s Inst i t ut e of

Technol ogy

Cambr i dge 39, Ma s s ,

At t n: Pr of . W. M. Rohsenow,

Dept . Mech. Engr .

Pr of . A. T. Ippen,

Hydr odynami cs Labor at or y

Mi chi gan St at e Col l ege

Hydr aul i cs La bor a t or y

Ea s t Lansi ng, Mi chi gan

At t n: Pr o f , H. R. ' IIenry

Uni ver s i t y of Mi chi gan

Ann Ar bor , Mi chi gan

At t n: Di r ect or , Engi neer i ng

Re s e a r c h Inst i t ut e

Pr of . V. k. St r e e t e r ,

Ci vi l Engi neer i ng Dept .

Uni ver s i t y of M~n n e s o t a

St . Arithony Fa l l s Hydraul i c L

Mi nneapol i s 14, Mi nnesot a

Attn: Dr . L. G. St r aub, Di r ,

New Yor k Uni ver s i t y

Inst i t ut e of Mat hemat i cal Sci ences

25 Waverl y Pl a c e

New Yor k 3, New Yor k

At t n: Pr of . R, Cour ant , a i r ,

(1)

Uni ver si t y of Not r e Da me

Col l ege of Engi neer i ng

Not r e Dame, Indi ana

~ t t r a : b e a n M. E, Schoeraherr

( I )

Pennsyl vani a St at e Uni ver s i t y

Or dnance Re s e a r c h Labor at or y

Uni ver si t y Pa r k , Penns yl vani a

Attn: Pr of . G. F. Wi s l i cenus (1)

Re ns s e l a e r Pol yt echni c Lnst.

Dept , of Mat hemat i cs

Tr oy, New Yor k

At t n: Dr , El i rsh Gohen (1)

St anf or d Uni ver s i t y

St anf or d, Cal i f or ni a

At t n: Appl i ed Mat h, and

St at i s t i cs Labor at or y

Pr of . P. R. Gar abedi an

(1)

Pr of . L. I. Schiff, Dept , of

(1)

Phys i c s

Pr of . J. K. Vennar d, Dept.

(1)

of Ci vi l Engi neer i ng (1)

St evens Inst i t ut e of Technol ogy

Exper i ment al Towi ng Ta nk

71 1 Hudson St r eet

Hoboken, New J e r s e y (1)

Wor ces t er Pol yt echni c I nst i t ut e

Al den Hydrat rl i c Labor at or y

Wor ces t er , Ma s s .

At t n: Pr of . J. L. Hooper ,

Di r ect or (1)

Dr . Th. von Ka r ma n

1051 S . Mar engo St r e e t

Pas adena, Cal i f or ni a (1)

Aer oj et Ge ne r a l Cor por at i on

6352 N. I r wi ndal e Avenue

Azusa, Cal i f or ni a

At t n: Mr . C. A, Gongwer

(1)

Dr . J. J. St oker

New Yor k Uni ver s i t y

I nst i t ut e of Mat hemat i cal Sci ences

25 Waver l y Pl a c e

New Yor k 3, New Yor k (1)

Pr of . G. C. Li n

Dept . of Mat hemat i cs

Mas s achus et t s I nst i t ut e of

Techno logy

Cambr i dge 39, Mas s .

(1)

Dr . Coburnbus I s el i n

Woods Eiole Oceanogr aphi c Inst .

Woods Hol e, Ma s s , (1)

Dr . A. 13, Ki neel , P r e s ,

Uni on Car bi de a n d Car bon Re -

s e a r c h Labor at or i es , Inc.

30 E. 42nd St .

New York, N. Y. 0 )

Dr . F. E. F o x

Cat hol i c Uni ver s i t y

Washi ngt on 17, D. C. (1)

D r . I mmanue 1 E s te r mann

Offi ce of Naval Re s e a r c h

Code 419

Navy Re par tnn en t

Washi ngt on 25, D. C.

Goodyear Ai r c r a f t Cor p.

Akr on 15, Ohio

At t n: Secur i t y Of f i cer (1)

Dr . F.V, Hunt

Di r e c t or Acous t i cs Re s e a r c h

Labor at or y

Ha r v a r d Uni ver s i t y

Cambr i dge, Ma s s . (1)

Pr of . Rober t Leonar d

Dept . of Phys i c s

Uni ver si t y of Cal i f or ni a a t

Lo s Angel es

Wes t Los Angel es, Cal i f. (1)

Pr of . R, E. H. Ra s mu s s e n

Euddenvej 47, Lyngl-~y

Copenhagen, Denr nar k

vi a: ONR, Pas adena, Cal i f. (1)

Techni cal Li br a r i a n

AVGO Manv. facturing Coxp,

2385 Re ve r e Beach Parkway

Ever et t 49, Ma s s ,

0)

Dr . L. Landv~ebes

Iowa I nst . of Hydr aul i c Research.

St at e Uni ver s i t y of Lawa

Iowa c i t y , Iowa (11

Dr, M. L, Ghai, Supervi sor

l i eat ~r a ns f e r / . Fl ui d Mechanics

Rocket Engine -Applied Resear ch

Building 600

Ai r cr af t Gas Tur bi ne Division

Gener al El ect r i c Company

Cincinnati 15, Ohio (11

Dr , W. W, Cl ausan

Rose Polytechnic Institute

R. R. No. 5

Te r r e tlaute, Indiana ( 4 )

Mr , Kur t Ber man

Rocket Engine Section

Ai r cr af t Gas Turbi ne

Development Dept.

Malta Te s t Station

Ballston Spa, New Uork

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