, 1

; I I
1
'1
I !!
:
. 1
t i
'1 1
~. !
Chapter 8
CENTRIFUGES
1 . IDSTORICAL INTRODUCTION
The effect of the earth's gravltattonal fleld on the eompostton of
the gases Inthe atmosphere at varlous helghts has long been recog-
nized. For, If PI ls the partal pressure of a gas of molecular welght
MI, accordlng to the Boltzmann dlstrlbutton law
( 6 . 1 )
where h t s the helght; g ls thegravltatlonal constant; R ls the gas
constant, 8. 31 4 x lO" ergsOK/mole; and T ls the absolute tempera-
ture. Then for two gases of dlfferent molecular welghts M
1
and MI
( 6 . 2 )
The suggestlon that gravltational or centrlfugal !lelds are suitable
for lsotope separation was made by Llndemann and Ast en' In 1 91 9.
Infact, they proposed that samples of neon taken at ground level and
at 1 00,000 ft would show a sensible shlft In tbe sot opt c abundance
ratio.
In a centrlfuge, vastly more powerful Helds are avallable. The
energy per mole at radius r in a centrifuge rotating wlth angular ve-
locity w ls ~Mi(wr)2. This expresslon for the energy replaces - MIgh
in Eq. 6 . 1 , givlng
( )
MI(wr)2
PI r =PI(O)exp 2RT
(6. 3)
I Phll. Mag. , 37: 530 (1 91 9).
1 03
1 04
THE THEORY OF ISOTOPE SEPARATION
Between the perlphery r =r
a
and axis r =O, for two dlfferent gases,
from Eq. 6. 3,
(6. 4)
where wr
2
ls the veloclty of the inslde wall of the rotor, the lnner
perlpheral veloclty.
In a blnary system, lf N ts the mole fractton of the sotope havlng
mass MI'
PI +PI =p.
N =pJp
1 - N =palp
(6. 5)
and p - p(r)ls the total pressure. Then Eq. 6. 4 becomes
(
--L) . (--!L) ex (MI - M2) (wrl)
1
- N 1 - N P . 2RT
r. o
( 6 . 6 )
It ls usual to take MI > MI' and accordingly
( 6 . 7 )
\
so that Eq. 8. 6 takes the form
)
where Qo t s the(equllibrium) simple-process factorof the separation.
The value of the simple-process factor for a peripheral veloclty of
300 meters/sec, T =300
o
K, and a mass dlfference of one unlt ts, by
Eq. 6. 6, Qo =1 . 01 83.
Shortly after the suggestlon of Llndemann and Aston was made
1
, at-
tempts were made, In rather crude apparatus, by Joly and Poole and
by Mulllken2 to reallze this separation factor, but these were unsue-
cessful. The Idea of the evaporative centrifuge was introduce~ a~t~e
time by Mulliken. In this method a small amount of ltqutd is
same h . h Dur
introduced lnto the centrifuge, forming a layer at t e per ip ery. -
1 Phll. Mag. , 39: 372 (1 920).
J. Am. Chem. soc. , 44: 1 033 (1 922).
__ " t 1u O ; ; -
__ rn vacuum-chamber centrifuges, which
_ _. nuraIlon and thermally lsolated to eliminate convec-
__ -"". n:urrents, flnal1 y permitted successful centrlfugalisotope separa-
tton to be obtalned In 1 939. Beams and Skarstrom
2
at the Unlversity
of Virginia, usng the evaporaUve centrl!uge method onCCI. . ,reported
a 1 3per ctmt change in the Cl
35
/Cl
37
ratio. Shortly thereafter Hum-
phreys,3 using the same technique on ethyl bromlde, altered the
Br'78/Br
81
abundance ratio by llper cent.
Thesimple-process factor of centrifuga} separatlon depends on1 y
onthe mass difference. Unlike other methods (e. g. , diffusion through
barriers, where a varles as AM/M) tt ts no more dIfficult for heavy
elements than for lght, Inaddt t on, t ls posslble to calculate a priorl
. tbe separat on to be expected from centrtugal apparatus wltbout any
undetermtned constants or tbeoretical uncertantes.
The simple-process "flow-through centrl!uge," as the concurrent
flowtype was called, ts an applicaUon to gaseous flow o the conUnu-
ous cream separator, As originally conceived, a single stream o
~as enters one end o a rotor through a hollow shaft, and two streams
,re taken off the other end, one Irom the periphery and the other near
'leaxis. This method produces a small change in conceiltratlon per
achine.
The countercurrent flow type was designed to attain considerable
oaratton in a single centr1 fuge, thus reduc1 ng the number of stages
i ured and the amount of material circulated between stages, As
~inally proposed by Urey," crculatton was to be established by
inuous distillation of UF8from the bottom cap of the rotor. The
r . was to be condensed on the top cap. 'The heavy liquid would
be forced out to the perlphery and would flowdownthe walls to
ottom cap, countercurrent to the vapor flow, and complete the
Bramley and Brewer
5
and Marttn and Kuhn' in Germany pro-
to establish countercurrent flow by thermal convectlon.
Modern Phys. , 1 0: 245 (1 938); Rev. Sel. Instruments, 9: 41 3 (1 938).
Rev. , 56: 266 (1 9391 .
Rev. , 56: 684 (l939).
s on Progress in Physies, VI: 72 (1 939).
1 , 92: 427 (1 940).
Ik. Chem. , A1 89: 21 9 (1 940).
_~",--. ,,--'''feX pOse the theory of centrifugal sepa-
_ ~. -YUiOU8 tYpes of centrl!uges. The important questlon of
- meehanical deslgn wll1 be dealt wlth only Inso lar as lt ls essentlal
to the understandlng 01 the process deslgn. The partlal differentlal
equatton 01 centrifugal aeparatlon la derlved 'In sec. 2. In sec, 3the
theoretlcal maximum separative power 01 a centrifuge i8found. The
solutlon for th evaporaUve centrl!uge ls glven In Seco 4, that lor
the concurrent centrifuge In see, 5, and that lor the countercurrent
centrifuge in Seco6. Sectlon 6 investigates at length the properUes 01
the countercurrent centrifuge.
The wrlter was lntroduced to the art of eentrifugatlon by C. Skar-
strom, formerly of tbeUnlveraUy 01 Virginia and later wlth theStand-
ard OU Development Campany. Harold C. Urey parUcipated actively
1 nthe early work, until bis other responsibutUes became too heavy,
contr1 buUng ideas and physlcal interpretaUons o mathematlcal re-
sults. Irving Kaplan shared in 1 . 1 1 the developments subsequent to
December 1 941 , notably the work on cascades o centrl!uges (in-
corporated largely in Chaps. 1 to 5) and the design problem
Z. PARTIAL DlFFERENTIAL EQUATlON OF CENTRIFUOE
As a preliminary to the derivaUon of the dl!ferenttal equatlon, con-
slder or a moment a centrifuge contalning a single pure gas. The
gas ts supposed to rotate uniformly at the same speed as the rotor,
t. e. , w radlans/sec; to have no other motons; and to be lsothermal.
Choose a cylindrlcal coordlnate system, rotattng wlth the gas, with
the origin at the axes oCrotatlon. The eUect of the rotatton ts to set
up a centrifugal force w
2
r per un1 t mass. Unde~the lnfluence this
force, a pressure radient isestablished according to the hydrody-
name equatlon
(6. 8)
Here pis the denslty of the gas mixture in grams per cubic centime-
ter. The quantUles p and pare related by the gas law
RTp
p"--
M
Combinlng Eqs. 8. 8 a"" It ,.
The denstty dlstrlbutlon (Eq. 6. 1 0), co!tsldered from a molecular
polnt of vlew, 1 8a dynamlc equtllbrlum between the effect of random
motlon of the molecules (dlffuslon), whlch tends to erase denstty
gradlents, and the effect of the centrlfugal fleld, whlch tries to pile a1 1
the molecules at the perlphery. The diffuslon counter to the density
gradlent glves a current densUy (in grams per seeond per square
cenUmeter)
ap Mw. r
-O-I O'-Op-
ar RT
Rere OIs the coefficlent of seU-difluslon. The outward current per
square centlnieter caused by theeentrlfugal force, which balances
tMs Inward current, must therefore be
(6. 1 1 )
In mixtures, Eq. 6. 1 1 holds for each component separately
(6. 1 2)
01 Isthe diffuslon eoeffielent for nioleeules of type 1 tbrough the whole
mixture. For Isotopie mixtures the exaet meanlng of the diffuslon
coefficlent Is of no slgnlf1 cance, and henceforth the subscrlpt w1 ll be
dropped. EquaUon 6. 1 2 ts the deslred expresslon for the flux of mole-
cules caused bya centrlfugal fleld, and U s now posslble to derive
the dlfferenUal equat on,
Conslder then a centrtuge contalnlng a perfect blnary gas mixture,
Isothermal and rotaUng uniformly. In order to accompl1 sh separa-
ton, the gas ts made to flow radla1 1 y and axia1 1 y. Interms of the
cylindrical coordinate system chosen as befare, the motion of the gas
as a whole (drift velocUy) is given by the compnents
(Radial) . u =u(r ,z)
(Azlmuthal) v =O
(Axial) w =w(r ,z)
Because of thls motion of the gas, the equUibrlum dlstrlbutlon (Eq.
6. 3 or 6. 1 0) Is conUnua1 1 y upset. The system moves material In an
effort to reestabllsh equ1 l1 brlum In thls way a transport of the de-
slred material 1 8set up,
1 07
1 08
THE THEORY OF 1 S0TOPE SEPARATI ON
Imagine a small annulaz reglon Inthe rotor, bounded by the cyl1 n-
ders r = ro and r ro + 6r and by the planes z =Zoand z = Zo+6z. In
a short Ume Interval 6t there flows across the cyl1 ndrlcal face r lO ro
an amount of deslred Isotope (denoted by the subscrt pt 1 ),
(6. 1 3)
In thls equaUon P1 u t s the flow caused by the drift velocity, PlUe. Is
the flow Impressed by the centrifugal fleld, -oapJar t s the con-
trlbuUorf from dlCfuslon agalnst the densUy gradlent, and 2lTro6z Is
the area of the cyl1 ndrlcal face. Llkewlse the flowacross the plane
face z =Zols
(6. 1 4)
The change Incontent of deslred material Inthe volume element t s
therefore
Introduclng Eq8. 6. 1 3 and 6. 1 4 t nt o 6. 1 5 and makng use of the rela-
tlon of Eq. 6. 1 2 for u
c
, (dropplng the subscrlpt O),
1 ( M w1 r e ) &(P1 w) O&I~l
~ "rDp ~ - D~ +P1u - + &
at - rir 1 RT &r az. z
(6. 1 6)
Now
MI' MI N
PI = RT PI =RT P
(6. 1 7)
and
(6. 1 8)
SubsUtuUng Eq. 6. 1 7 In Eq. 6. 1 6, ustng Eq. 6. 1 8 and notlctng that Op
=constant, tt 1 8found that
CENTRIFUGES
~ =. QE. -!. [r ~ + (MI - M,)wlr
a
N(l - N)]
P at r lr ar' RT
1 l l . al
- r ar (Npru) - az (Npw) +D aza (. Np) (6. 1 9)
whtch s the destred parUal differenUal equat on of centrifugal sepa-
raton,
The three ktnds of centrifuge descrtbed In Sec. 1 are governed by
speclal cases of Eq. 6. 1 9. In the evaporaUve centrifuge w =Oand
ru :: constant ln the concurrent and countercurrent centrifuges u =O,
and w descrlbes the respecUve types of flow. The solutlon of Eq.
6. 1 9 for these cases t s the subject of the subsequent sect t ons devoted
to the particular centrlfuge types.
3. MAX IMUM SEPARATIVE POWER OF A CENTRIFUGE
Inthls section the maxtmum separative work that can be performed
by a centrifuge' wUl be determined. It wUl be used as a standard to
evaluate the efftclency of the vart ous centrifuge desi gna,
Uslng the result of Seco6 (Eq. 1 . 60),
(T- NP) (N' - N)
6U = N2 (1 - N)2
The net transport oi desired material (in moles per second) across a
suriace element do s, accordlng to the analysls given n a precedlng
secton,
(6. 20)
where ro t s a unit vector along a radlus t hroughdou
el
t s the vector
velocity created by the centrifugal field directed along ro and w1 th
magnitude glven by Eq. 6. 1 2, and the symbol V t s the vector gradlent
operator.
Thus the separative power for a small slab of tblckness ds, with
faces do normal to VNand sldes parallel to VN, t s
dU ~Dp
RT
(6. 21 )
I Followlng Dlrac.
1 09
1 1 0
THE THEORY OF rsOTOPE SEPARATION
The symbol lndlcates the scalar producto
Taklng VNas a variable and da ds and everythlng el se constant,
Eq. 6. 21 t s a maxlmum when
1 w1 r ).
VN T (MI - Ma) RT N(l - N ro
that ts, along the dlrecUon of the centrifugal neld, and one-half tbe
equtllbrlum value. Then
(8. 22)
(dU)
Dp [(Ma - M,)wlr]1 do dr
max - RT 2RT
IntegraUng over the whole centrifuge, of length Z and radlus ra'
(6U)m&ll _ J (dU)m&ll _ ~~ [(Ma ;~,)Wl ri
r,
r
l
2uZ dr
Dp [(Ma- M,) (wrl>,]1 . Z (moles/see)
-1 ff 2RT 2

[
(Ma - M,) (wr. ). ] . Z (grams/see)
-pD 2RT 2
(6. 23)
Note that the expresslon In brackets ls the exponent of ao (Eq. 6. 7)i
The mt. nlmum number of centrifuges oi length Z and perlphera
veloctty wr requlred to perform a glven separaUon ls, by Eqs. 1 . 44
and 6. 23, AU/(6U)max' The value of (6U)maxdependa on the perlPhera~
veloctty of the fourth power, whlch puts a premlum on hlgh perlph
eral veloclties. The separative power ls a~so proportlonal 'lo the
length. But for constant peripheral veloctty, the separation ls I n-
or
wl, . . . !.
p
where T la lbe atreaa in lbe wall and pta Ita denstty. The rotor wUl break when T
pwl rI la greater tban the tenaUe etrength of a metal.
CENTRIFUGES
dependent of the radtus. The radlus affects the holdup and in t
current centrifuges the flow lnto the rotors, but ls o~herwls:~~e~:=
vant. It t s usually chosen by mechanlcal conslderaUons.
SURFACE dc: r
\
\
\
\
\ /t
\ I
m
\'t'/
\ I
V
(0. )
(b)
Pig. lU-Stresses iaath1 taU ' dlagram. aro ngcyUnder. <a)Stress~ laawallsector. (b)Vector
4. THE EVAPORATIVE CENTRIFUGE
In the evaporative centrifuge N t s lnd d
slderlng the steady state, aN/ at =OandeEpeqn 6
en
1
t
9' of d
Z
'and w '" O. Con-
re uces to
~ :r {DP [r ~~ +2AAr N(l - N)] - NPru} ;: O
\
where
(6. 24)
(6. 25)
1 1 1
1 1 2
THE THEORY OF ISOTOPE SEPARATION
8uppose vapor ls removed from the axts at arate L moles/seco
Then
- :T 2wrZu = L (8. 26)
Multtplylng Eq. 6. 24 by the constant 2,. . Z/RT and ntegrattng,
(6. 27)
where
" 27rZ~~ (moles/s
ec
)
(6. 28)
The lntegraUon constant was evaluated by noUng that the left slde o
Eq. 6. 27 vanlshes at r '" O. '
Replaclng N by R as dependent variable,
(
aR ') l 1 l R -R(O)l
" r ar +2AAr R = L R(O) - R(r) 1 + 1 +R(O)
(6. 29)
R -R(O) .
Now 1 +R(O)'lE - AAra N(O), whtch can be neglected with respect to
untty. After thus slmplifylng Eq. 6. 29, the solution t s readUy found to
be
and o~lntroduclng Eq. 6. 7, whlch Interms of AA t s
\
(6. 30)
tMs' expresslon may be wrltten
R(O) =R(r
2
)Oo(2::L)
(6. 31 )
Equation 8. 31 glves the relation for mole fractton ofproduct N(O)
In terms of the composlUon of the charge N(ra) and the rate of pro-
'~
I , . ~
1
1
]
CENTRIFUGES
1 1 3
duetton,' If tt la aaaumed that the production la only a small Iractton
of the charge, or that successlve batches o{product are kept separate,
the separative power of the centrlfuge Is (ct . Appendlx D)
(6. 32)
The value o{6U s a maxlmum when L =2 ' Y :
(6. 33)
whlch t s the same as the theoreUcal maxlmum separative power of a
centrlfuge (Eq. 6. 23).
Inthe development [ust glventhe gas was assumed tobe Isothermal.
Thls -pcture Is far too simple. When vapor ts wlthdrawn at the axis,
the gas cools by' expanslon and a temperature gradlent t s Induced.
The gradlent ts determlned by the balance between the rate of cooltng
of the gas and thermal conductlvlty. As L Increases, the gradent
increases until the gas reaches the dew pot nt or the adiabaUc gra-
dent , The mean effective temperature Teff t s therefore reduced as a
function of L.
An attempt may l1 e made to account for this effect by writing in
place of Eq. 6. 31
(6. 34)
Slnce T/T eff Increases wlth L, the ssparaton wll1 not {al1 off quite so
fast with L Inpractice as Eq. 6. 31 would tndcate,
A unlt welght ogas rotatlng near the perlphery with angular ve-'
loelty w has the angular momentum r~w; at the'axis tt has none. When
gas Is moved from the periphery toward the axis, means must be
provided to absorb this excess angular momentum, which otherwise
tends to Increasethe angular velocity of the gas at smaller radlt,
This is accomplished by radial baffles
2
(lookng downalong the axis,
a star) which prevent the gas from rotating at angular velocities df -
ferent from that of the rotor. .
1 Thls result was foundby Humphreys, Phys. Rev. , 56: 684(1 939).
a Beams andSkarstrom, Phys. Rev. , 56: 266(1 939).
1 1 4
THE THEORY OF ISOTOPE SEPARATION
Although the evaporattve centrlfuge~ wtth L =2", delivers 1 00per
cent of the theorettcal separatlve power, lt ts not easlly adapted to
continuouS operaUon.
5. THE CONCURRENT CENTRIFUGE
Llke the evaporattve centrlfuge, the concurrent centrifuge ls a
slmple-process machlne slnce the enrlchment factor per machlne ts
lhnlted to ao'
Inthls devlce axial flow ls used to obtaln an axial as wel1 as a ra-
dial concentratton gradlent. The gas enters (Flg. 6. 2) Intwo streams
at one end of the rotor and flows axially to the other end, where the
streams are removed separately. Durlng the passage through the
centrlfuge the streams tend to assume the (radial) equtlibrlum dt s-
trlbution (Eq. 6. 6). The flow pattern adopted {or the concurrent cen-
trifuge conslsts o two thln cyllndrlcal streams located at radll r
i
and r (perlphery) andflowlng parallel to the z axis. (The opUmum
positton ior the t nner stream t s not at the axis, as wll1 be seen sub-
sequently. ) There t s no radial mass flow.
A rotor wlth a double entrance (so that entering streams of two
different concentrattons can be used) will be considered; prevlously
theliterature has covered only single-entrance machines. Thedouble-
entrance centrifuge ts more flexible than the tatter. Cascades of
these elements, whlch are more general than the element of Chaps. 1
to 5, are studled Indetall InAppendlx E. Among the more lnteresting
featureq of thls study t s the result that the no-mixing case (both
entering streams of the same composition) is not an opt t mum.
The solution given here follows roughly the demonstraUon by Mur-
phree, whlch for the case considered t s superior to the more general
method t hat was originally used. The value of u is zero, and the flows
are generally so large that ba(:k-diffusion ts negligible. Then Eq. 6. 1 9
reduces for the steady state to
O: : Dp . !-(r ~ +2AAr N{l - N)] - -aa (Npw)
r ar ar z
(6. 35)
In the reglon between r = r
i
and r = r
a
, w = O, so that Eq. 6~35inte-
grates to
_-P. . 2lT[r ~ +2AAr
l
N{l - N)] !(Z)
RT Sr
(6. 36)
GAS EXI T
1
J
1 1 CAP
I ll
i
z o z
1
t
\
1
1
1
~. .
ROTOR WALL
'f
1
I
'4
CENTRlFUGES
I I I "'--SHAFT
1 1 5
zoO
rll. 1 I. 2-Slmpl. madelof aasICua concurrent c. ntrltu,
1 1 8
THE THEORY O, ISOTOPE SEPARATION
where f (z) ti the tranlport 01 dellred tlOtOpe acrol. a cyllndrlcal
element 01 unlt length between the two atream
But also, tf L(r. ) 1 1 the flow ln the Itream at r r. ,
(6. 3'7)
and
L(r. ) N(r. ,z) + L(rl)\N(rllz) L(r. ) N(r. ,O) +L(rl) N(rllO)
B (a constant> (6. 38)
Integratlng Eq. 6. 36 between r
l
and r. , constdertng AA N(1 - N)
constant to terma 01 the order 01 (AA)',
_ ~ III(N(r. ,I) - N(r"l) +AA,(rl-l1 ) N(l - N) f (1 )In t (8.39)
and substttutlng lor f (z) from Eq. 6. 3'7 and for N(r"z) from Eq. 8. 38,
~~ 21 1 [ ~. - N(r
l
) (1 +i:-) +AA(ra- 1 1 )NU - N)]
d r
= L
1
-d N(r
l
) ln. :. J.
z rl
IntegraUng thts ordtnary dtfferentlal equaUon for N(ru
z
) and re-
arranglng the result,
N(ruz) - N(rllO) = (1 - 9) (N(r. ,O) - N(rl,O)
+AA(r: - r~) NU - N)] (l - e-
ba
)
N(r"z) - N(r. ,O) - 9[N(r. ,O) - N(r,O)
+AA(r: - r~) NU - N)] U - e-
ba
)
(6. 40)
where
(6. 41 )
CENTRlFUGES
Th, ~eparatlv, power when N(r. ,O) and N(ruO) ar, molt favorably
r,lat,d 1 1 , accordln, lo Bq. 1 1 o Appendlx B,
6U[L(r. )+L(r. )) 8(1 - 8)(1 - e
obl
) (ln a )' (1 - 4 . )1
2 <t +eobS) o ~
, 1
and the separat~ve power per unlt length ls
!!!. . . ZODP(ln l' (1 - ) (-jr
z RT ~ bzb +e061 ) , \
l n " i t
whleh ls a maxlmum wlth res t lo /
ra/r 0. 534, pee r. r, for any value of bz when
!!!. . 21 rDp (1 - ,obl)
z RT (lnao) bz(1 +,. 6. ) 0. 40724
and a relatlve maxlmum wlth respeet tobz when bz lO O, namely,
('ZU}mu . 0. 407241 1 ' ~~ (t n(0)1 (6. 42)
If thls result ls eomp d lth are w Eq. 6. 23, tt ls seen that thls ls 81 45
per cent of the theoretlcal efflelency.
_ For a single entranee centrlfuge, lt ls neeessary te take N r O
dl~(~l'O). The separatlve power ls then, aeeordlng to Eq. 8of A;;n~
,
6U [L(r. ' +L(r. )] 9(1
2
-, 9)(1 - e
obl
)' (ln ao)' (1 - * r
and per unt length
'N( O) ( e
k
r. , - N rilO) - -; e: b& AA(r: - t1 ) NU - N)
1 1 7
1 1 8
THE THEORY OF ISOTOPE SEPARATION
Tbe maxlmum wlth respect to r/r, ls the same as before. The ex-
presslon1 (1 - eoba)I/bz has a true maxlmum at bz lO 1 . 25643 and thus
(
. !!!. ) (0. 40724)' 27rDp(In(Jo)'
Z ma. RT
(6. 43)
. whlch has an effleleney of 66. 34 per eent. The eondltlon bz 1 . 25643
glv;,:= iadeftnlte relatlon between the length of tbe rotor and the flow,
namely,
47rDp z
L. +L 1 . 5786RT 9'<t - 8)
(6. 44)
if lt ls remembered that the separative power IS the product of the
concentratlon difference and the transport, the maximum of 6U wlth
respect to r/r, is easily understandable. The concentratlon differ-
ence t s the maximum when r/r, =O, but the transport (through the
eyUnder of radt us zero) is zero. The transport ls a maxlmum when
rl/r 1 , but the coneentraUon differenee is zero. The maxlmum of
the product thus Ues somewhere Inbetween.
. A fuller discusslon of the significanee of the dependence of the re-
sults on 1 _ e-bl, the degree of equUibrium attained, t s given in Ap-
pendix E. The phenomenon Is a quite general one.
NoUce that b contains the factor 9(1 - 9) (L1 +La)' Decreasing
9(1 _ 9) and lncreaslng L
I
+L, leaves thls factor unchanged, but small
total flows are deslrable and 9(1 - 9) should obvlously be made as
large as posslble, which requires 9 =Ya (cf. Eq. 6. 44).
Further properttes" of the coneurrent centrifuges may be obtained
from the equatlonsglven.
1 Note that the correspondence e-k - t1 /r: maltes thls talte the lorm
Ut
In "i t
1
. For example, lor any r!r. the dependence on z/(L +Lj ts the same, and the
maxlmum lor the stngle entrance centrlfuge la at the sa~e place, bz 1 . 256 [wtth the
approprlate value of ln (r. /r,) Inb]. But for z/(L1 +L. ) preasslgned (and not bz) the
maxlmum wtth respect to r!r. varles.
CENTRIFUGES
8. THE COUNTERCURRENT CENTRIFUOE
Countercurrent separatlng devlces Ingeneral have the property o
multtplylng the equUlbrlum slmple-process factor many Umes in one
untt. Because of the nature of the flow, a concentratlon gradlent whose
slze t s Umtted only by back-dlffuslonls estabUshed in the dlrectton
of the flow.
Slnce a large separatton ls obtalnedln one untt, much of the recy-
clng between untts whlch ls otherwlse necessary to multlply the stm-
ple-process factor ls avolded. Furthermore, the problem of cascade
operatton ls very eonsderably slmpUfled slnce the number of untts
Inseries requlred to effectuate a given fracttonatton decreases enor-
mously. The cascade becomes broad lnstead of long and t s easUy
broken down into lndependent parallel sections. Countercurrent flow
Is also efficient from a process standpoint because it is possible to
maintain maxhnum separative power through the entire unt , "For all
these reasons, which have long been appreciated by chemical engi-
neers, countercurrent processes are preferred if at aH possible.
The dlfferenttal expresslon of Eq. 6. 1 9 becomes for the counter-
current centrifuge
aN Dp a [ aN ] aN a
2
N
p - = - - r - +2~Ar2 N(l - N) - pw(r) - +Dp --
st . r ar ar az az
2
(6,45)
The solution of Eq. 6. 45 may be ound by foHowlngtbe standard meth-
ods for soluton of partial differentlal equatlons, Thls method was
utilized In lune and luly of 1 940. However, Eq. 6. 45 s particularly
simple stnce the gradients of the concentratlon Inall dlrectlons are
small. Thus the equat on for a countercurrent centr ugal column can
also be solved by the method used by Furry, Jones, and Onsager" for
the thermal-diffusion column. This pos~ibiltty was first pointed out,
and partially worked out, by Bramley. " A sim'Uar procedure was
employed by Martin and Kuhn. "
The results of the two methods are of course dentcal, The second
method will be demonstrated here because tt s easier and because it
'Incontrast to. concurrent devlces, In which aN/ ar cbanges w1 thz, 80 that fthe
separaUve power ts an opUmumIn one place 1 t Is necessarUy less In every other
place.
a Phys. Rev. , 55: 1 083(1 939).
a Sclence, 92: 427(1 940).
Z. physlk. Chem. , A1 89: 21 9(1 940).
1 1 9
The integratton constant (a function of z and t) was e~aluated ~y re-
membering that r( aN/ ar) - O as r - O.
The second integration wtth respect to r requires a little more
. artiflce in order to get a form ln whlch the lntegration constant can
be evaluated. The boundary condltlons are
Equatton 6. 48 may be tranSformed by lntegrating by parts the flrst
term on the left-hand side,
( i
t. pw (t. aN dr i
t
PRw
T
r dr)
271 :z N(r2,z) o RT r dr - Jo ar . o
_ 2 . !- t. Dp ~ r dr - 21 1I
t
.LaN r dr (6. 49)
- 1 1 az o RT az o RT at .
Equatlon' 6. 49, although lt does not glve the lntegra:tlon constant that
would permlt the integratlon of aN/ ar ltself, tells howto lntegrate
1 20
THE THEORY OF ISOTOPE SEPARATION
permlts the case in whlch the mole fractlon of the product ls large lo
be lncluded wlthout added compUcatlons.
The method depends essentlally on the fact that aN/ar ls of the
order of N(l - N)2AAr, whlch ls a small quantlty. Thus the varlatlon
of N with respect to r, as compared to the varlatlon of r, p, or pw,
may be neglected. For example
f
~ pw r dr - aN f pwr dr +terms of the order of AA
2
az az
Consequently Eq. 6. 45 may be integrated with respect to r, The flrst
lntegration gives directly, dropplng alN/ az
l
and aN/ at, which are o
second order.
a
N 1 aN I
t
pw
_ =-2AAr N(l - N) +- - - r dr
ar r az o Dp
(6. 46)
.
(6. 47)
CENTRIFUGES
!
I
I
. .
lNl' pwr dr, whlch Is [ust as useful for preaent purposes. SubsU-
lr o
tutlng Eq. 6. 46 InEq. 6. 49, lt la found that
(6. 50)
where
271 (M; - M1 )w
2
1" l'
C
l
=RT RT o r dr o pw r dr
21 1 ' 1 1 " dr (I ' )1
Ca - -. - pw r dr
RT Dp o r o
(6. 51 )
2 11' L
c. = RT o pr dr = holdup per unlt lengtb (moles/cm)
Equatlon 6. 50 has the form of Eq. 2. 1 , the typlcal equatlon for t so-
tope separatlon In a square cascade or eolumn, The propertles of
such columns, lndlvldually and Incascades, for fixed values f c
l
, c
s
,
and c. were studled In Chaps. 2, 3, and 4. The followlng dlscusslon
covers the investlgatlon of howthese coefficlents vary as a result of
changes Inoperatlng condt ons, The material 1 1 1the earlier chapters
will be referred to constantly.
In order to examine propertles of the countercurrent centrifuge,
attentlon will be confined for the moment to a single centrifuge. For
convenience it will also be assumedthat N<l, althou~h this is by no
means essential to the argumento Then the steady-state solutton of
Eq. 6. 50 is (Eq. 2. 1 4)
N(Z) 1 +r/ J exp [2EZ(l +lP)]_ (1 +lP)e2cS(l+ljI)
N(O) = 1 +lP exp [2EZ(l +lP)] - 1 +lPe2cS(l+ojI)
1 21
1 22 THE THEORY Ol' mOTOPE BEPARATlUN

where
P PRT
lPe; 21 r(M - M ) . w
l
I r . r dr i' pwr dr
I 1 RT O O
(M - M)w
2
1" r dr Ir pwr dr
I 1 RT O O
2E =~ = -1 -l-f' dr (I ' pwr dr) 2
Dp 2 + Dp o. ro'
(6. 52)
. d th f cUon pw whlch measures
The quantlties cland cadepen on e u~ do~the flow pattern,
the up-and-down flow, Intwo ways: They epen nthe absolute
or the locatlons and relative slze o the streams, and o b the post-
magnltude o the flow. The pattern ts butlt lnto(the:oto~e)y o baffles.
tlon of oriflces In the end caps and posttton or a sen be ad-
But the magnltude of the flow t s an oper~t~~~:::~:b~::~~t~~~al con-
justed from outslde. Thls lndepednden~eif ge gives lt more flexlbility
strucUon Ina properly conceive cen r u
than the otherwlse analogous thermal-diffuslon column,
Therefore a newquantity L t s lntroduced.
L=; ; ['. [pw] r dr
(6. 53)
whlch ts the flow up the column plus the flow down the column, Then
I
rpw r dr
O L
does not depend on L, and Eq. 6. 52 becomes
P
lP= -
alL
_ a1 L
2E - e +a La
2 a
/L
d c,/L
1
do not vary wlth L.
where al Clan a, f L and . /. For any value
N(Z)/N(O) 'la now a functlon o '1 "
h the rate of production t s zero.
N(Z)/N(O) ls greatest w en
N(Z) = exp ( a1 L z)
N(O) ca+aa
L2
(6. 54)
of L,
Then
(6. 55)
CENTRIFUGES
1 2 3
and the maxlmum posslble valu f ()/
centrifuge and 1 t e o N Z N(O) or a glven length o
or a gven ype o countercurrent !low ls
(6. 56)
",here 2E
o
ls the maxlmum o a,L
c
I
+a,L1 wlth respect to L and la
(6. 57)
Thecorrespondlng value o L t s
(
DP) I rl
Lo = &. = 27Tr 2 RT o I pwI r dr
Va; J2 I rldr (I r )2
O r O pwr dr
(6. 58)
The exlstence o a maxmum In E t s h
enon o back-diffuslon . Th P yslca1 1 y due to the phenom-
E. When L, the total fl~w in~h:o~ce~t~atlon gradient ls proportlonal to
ton gradlent Is sma1 1 , back-dus uge, is large and the concentra-
E varies lnversely as L But on ts negliglble (e, <: a,L
I
) and
. as soon as L ts small a d d
centratlon gradient are largeb k d n Ean the con-
flna1 1
Y
. limltlng the attainable'fr;~tl~n~:~:~~n plays an lmportant role,
It wtll be found convenient to measure 1 1 fl
Therefore set a ows In terms of Lo.
L
m=-
Lo
(6. 59)
Substituting in E,
N(Z) (l +I/ J) exp [2E
o
Z 2m (
_ _ +__~ : . : !+: . . !r: !!. a: . . . : . . l: : . . +. : . . . : I /J )l
N(O) =
1 +I/ J exp 2EoZ 1 ~mm2(1 +I/ J) ]
In terms o the dlmensionless parameters mand . 1 . P 1 gi
Y", S ven as
P =ml/JP
o
(6. 60)
(6. 61 )
1 24
THE THEORY OF ISOTOPE SEPARATION
where
P 4
2 Dp
0
= 7TE
o
r-
2 RT
(6. 62)
EquaUons 6. 57 to 6. 62 constltute a complete descriptlon o the be-
havior o the countercurrent centrifuge. When the type o now pwis
specifled, E
o
, Lo, and Poare determined. L and Pare the conditlons
lmposed and are measured on flowmeters by the experlmenter. By
Eqs. 6. 59 and 6. 61 , m and r/J are thereforeknown. Andfinally, sub-
stituting E
o
, m, and r/J In Eq. 6. 60, the fractlonation of the column 1 8
predictable.
The maximum separaUon factor occurs at L =Lo,but thls ls clearly
not the most efficient circulation rateirom the standpoint o separa-
Uve power, slnce the parasltlc phenomenon of back-dUusion t s very
lmportant at thls ow, The relaUve weight of back-dlffusion is re-
duced by lncreasing L (thus decreaslng the concentration gradent ),
These qualltative conslderations are contrmed by examining cm.
From Eq. 2. 33,'
su = 5. . . Z = a~L2Z I -. 5- Z(~) - 5- Z(~) (6. 63)
4c, 4(c
I
+ a,L ) - 4a, 1 + mI - 4c, 1 + mI
whose largest value t s reached asymptotically as m- ".
It should be noticed that thellmlting value oi 6U t s approached very
rapldly: When m=3 the separative power t s 90 per cent, and when
m=5 lt ls 96per cent oi c~Z/ 4c,. At these values of mthe concentra-
tlon gradient ls 60 and 38 per cent, respectively, o the maxt mum. !
Thus lt ls not necessary to dlscard the advantages o large separa-
tion ln one unlt, or to lncrease the flows lnordlnately, to get adequate
separation efflclency.
REFERENCES
Bramley, A. , The Centrlfugal Separator, Oct. 7, 1 940.
Cohen, K. , Report A-54, october 1 940; Report A-52, Jan. 21 , 1 941 ; Report A-50, Jan.
30, 1 941 .
'Conslstent wlth lhe earller sectlonsof lhls chapler,lhe symbol 6U ls b. lng used for
the total separatlv. pow. r, and not the separatlvepower per unlt lenglh as InChapo2,
Sec. 3.
"Th. factor 1 82m/U +mi).
CENTRIFUGES 1 25
Cahen, K. , memorandum lo H. C. Urey, May 1 4, 1940.
Cahen, K. , and l. Kaplan, Report A-I0l, lan. 28, 1 942.
Cahen, K. , and C. Skarstrom, Columbia Ser. No. 4R-X 1 38, Feb. 8, 1 941 .
Dlrac, P. A. M. , Brltlsb MS, 1 941 .
Ka~lan, t. , and K. Cohen, Report A-1 95, lune 1 7, 1 942.
Murphree, E. V. , Separatlan of Gases by Dlffuslonal Metbods, February 1 942
.
.