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ORNL-TM-2245.txt
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ORNL-TM-2245.txt
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et b
' iiifl -oafi -::-.i ‘l.
\.'.
Y
OAK RIDGE NATIONAI. LABORATORY
~ operated by
UNION CARBIDE CORPORATION
| NUCLEAR DIVISION - S
. for the
us. ATOMIC.ENERGY COMMISSION |
ORNL-TM- 2245
COPY NO.--.V 86
| -_DATE - July 23, 1968
F. N. Peebles -
' 'ABSTRACT :
Removal of dissolved Xenon-135 by mess transfer to helium bubbles
‘offers an attractive means of controlling the Xenon-135 poison level
in molten salt breeder reactors (MSBER's). In order to provide neces-
| sary engineering information for evaluetion of the proposed method, the:*
existing date on rates of mess transfer to ges bubbles ‘have been: -
'reviewed
. Rather extensive literature references point to reliable equations
for prediction of mass transfer rates to single bubblee,‘ising in '
stationary liquids under the two extreme cases of a rigid bubble inter-
- face and of & perfectly mobile bubble interface. In general, experi-
" mentel deta ere availsble which support these predictions. No relisble
criterion for predicting the transition from one. type behavior to
-another is available. o s S :
- An_elementary analyais'of‘the'ratee_of mass tranefer'to'bubblesl
cerried along by turbulent liquid in & pipe is presented. The results
indicate that the bubble mass trensfer coefficlent for 0.02 in.
- diemeter bubbles will be epproximately 13 ft/hr for mobile-interface
'rbubbles, end approximately 2 ft/hr for rigid-interfece bubbles. An
experiment is suggested to. provide specific data on the mass transfer
.retes to bubbles carried aslong by turbulent liquid 1n & pipe for hydro-
fdynamic conditions Wthh simulate the MSBR._-
ROTICE This document. contains information of ‘o preliminary nature .
and was prepared primorily for internal use at the Oak Ridge National
~ Laboratory. It is subject to revision or correcnon and therefore does .
not represent a final report. oo :
-
RO OF TS DOCUNM 1S UNURTER
LEGAL NOTICE -
This raporl was preparad as an occounf of Govarnmnf sponsorod work. Nmther tho Unn‘ed S!crres,
nor the Comn‘ussmn, nor any person acting on behalf of the Commission:
A, Mokes any warranty or represonfutlon, expressed or implied, ‘with respect to iho dcecuracy,
" completeness, or usefulness. of the information contained in this report, or that the use of -
any informatien, apparatus, methed, of process disclosed in this report may not infrings
privately owned rights; or
B. Assumes ony lichilities with- respect to the use of, or for dumages resulhng from the use of -
any information, apparatus, methed, or process dlsc!osod in this report.
~ As used in the above, “‘person acting.
on behalf of the Commlssmn" includes any employee ,of
‘eontractor of the Comrmsswn, of omp!oyee of such centractor, to the extent that such cmployoe
-or contractor of the Commission, or employee of such contractor prepares, dlssemmdies or
‘Vprowdos access to, any information pursucnf to !'us empioymenf or contract wnh the Commission, =
“of his omployment with such centracter,’
R T A e e
R T RAspaR RS AR et 4
)
-,
~
'fla.(""‘f
+
v CONTENTS
Page
Abstract 1
1.0 Introduction 5
2.0 Mass Transfer Theory ‘ 5
2.1 Mass Transfer Coefficients for Spherical Bubbles 9
Rigid Interface Case 13
Mobile Interface Case 14
2.2 Experimental Data on Mass Trangfer Coefficients 17
to Single Bubbles
2.3 Mess Trensfer Coefficients for Bubbles Carried 20
) Along by Turbulent Liquid
4 3.0 Proposed Mass Transfer Experiment to Simulate MSBR 25
) Contact Conditions
L.0 Conclusions 30
References Cited 32
LEGAL NOTICE
This report was prepared as an account of Government sponsored work. Neither the United
States, nor the Commission, nor any person acting on behalf of the Commission:
) A. Makes any warranty or representation, expreszed or implied, with respect to the accu-
- racy, completeness, or usefulness of the information contained in this report, or that the use
of any information, apparatus, method, or process discloged in this report may not infringe
privately ovned rights; or
B. Assumes any liabilitles with respect to the use of, or for damages resulting from the
- use of any Information, apparatus, method, or process disclosed in this report.
As used in the above, *‘person acting on behalf of the Commission® includes any em-
ployee or contractor of the Commission, or employee of such contractor, to the extent that
such employee or contractor of the Commission, or employee of such contractor prepares,
_ disseminates, or provides access to, any information pursuant to his employment or contract
" with the Commission, or his employment with such centractor. -
)
QISTREUTON OF THIS HOCUMENS @ ONL
»
L)
REMOVAL OF XENON-135 FROM CIRCULATING FUEL SALT OF THE-MSBR
BY MASS TRANSFER TO HELIUM BUBBLES
1.0 Introduction |
A pr0posed'method10 of removing XenonQiBS from the fuel salt in the
Molten Selt Breeder Reactor (MSBR) involves circuletion of helium bubbles
with the liquid fuel. Bubbles ere to be injected into the flowing stream
near the pump, and then dissolved Xenon—135‘is removed from the liquid.
" by mess transfer (combined diffusion and convection) into the bubbles.
The circulaeting bubbles are then to be removed from the liquid at the
outlet of the heat exchanger by a centrifugel separator.
Although the potentisl for Xenon-135 removel by mass transfer to
helium bubbles is high, the actual effectiveness of removal is controlled
by the surface area of the bubbles exposed to the liquid and the mass
transfer coefficient between bubbles and liquid flowing cocurrently in.
e pipe. This report deals with the.bubblevnass‘transfer rete expected
under the MSBR operating conditions, based on the information available
in the literature, and & proposed experiment to provide additional detsa.
The experiment involves simulation of the reactor flow and mass transfer
conditions through use of a glycerine solution es the liquid, oxygen as
the solute gss, and helium as-the stripping medium,
2.0 Mass Trensfer Theory
The esgsential features of the mass transfer situation of interest
is shown in Figure 1. Liquid flowiné along & pipe at the rate QL enters
the system with -dissolved concentra.tion, I1° end the inlet stripping gas
-at a flow rate, QG, is 1nJected into ‘the liquid. As the liquid.end gas
streams move cocurrently slong the pipe the dissolved ges content of - the
liquid is reduced to the exit concentra.tion,‘cL2
For-e& steady gtate system, conservation of the. dissolved ges .requires
thet the concentration change in accord with
% (cLl L).: 8 %> (1)
’(/,-Pipeline Contactor, Length = L, Croés Section = A,
ORNL-Dvg 68-6780
U Oy
Liquid Flow
&
QQ‘
e QL, r.CL -
|
QG,'Gas Flow Rate
Fig. 1. Flow Diagram for Pipeliné Contactor..
G2
. [ ™
N
-)
- where C
7
G represents the local concentration of the solute geas in the
bulk bubble stream. Equation (1) is based on the case of negligible
solute gas in the inlet stripping ges.
At eny location aslong the contactor, the concentration of dissolved
gas in the vicinity of the-liquid;gas interface of a typical bubble is
depicted in Figure 2. The:solute gas concentration difference between
thet of the bulk liquid and the liquid et the interface provides the
driving force for mass transfer at the rate,
e
RTQL
-, dp =K e &, (s Ec;g‘" Fa L] (2)
where
KL = liquid phaese mass. transfer coefficient,
e = gas-liquid. interfecial area per unit volumn of contactor,
AC = contactor cross-section,
dL = differentiel length of contactor,
T = absolute temperature,
R = universal ges constant,
H = Henry's lew constent for solute ges.
Equation (2) results from the clessic assumption of negligible interfacial
resistance,z and the assumption of small ges-phese resistence to mass
transfer. The latter assumption is en approximation which is eppropriate
for the case of & gas having & low solubility in the liquid of interest.
When Equetion (2) is integrated-to give the change in solute gas concen-
tretion over the total length of the liquid-gas contactor, it is found thet
C - -8
L2 o+ e
e ot e (3)
CLl l+a
K, & AL (1 + a)
where o = =——— gand B = —_
o HQG | QL | |
e e R | - 1 - %o
If the effectiveness for solute gas removal 1s expressed as E = —c >
SRR e R e 11
then for & given mass transfer system theieffectiveneés_fpr golute removel
is given.by _
3 -
_l~e
E==57—> (L)
ORNL-Dvg 68-6761 "
btk Tiqut tiquid.ces
‘Bulk Liquid - Interface
"
C.
- Bulk Ges G
For Negligible Gas Phase Resistance,
a1 = G
. Fig. 2. Concentration Profiles Near Interface..-
fl(: s
»
9
The maximnm,ralue of E is for a liquid-gas contactor of infinite volume,
1
l+o0 °
or infinite msss transfer coefficient, and is EMax
Figure 3 shows a plot of the Xenon-135 removel effectiveness ags e
function of liquid phese mess transfer coefficient for the MSER operating
conditions and helium bubbles 0.02 in. dismeter. The plot illustrates
_that the effectiveness for Xenon-135 removel is sherply related to the
liquid: phase me.ss transfer coefficient in the renge of 1 < KL < 100 ft/hr.
Kedlll has shown that the Xenon-135 ‘poison fraction in the MSBR is
influenced in en importent way by the bubble stripplng effectiveness, and"
hence successful reactorfanalysis‘and design for the.MSBR depends on rether
accurate_knouledge'of.the bubble mass'transfer-coefficient.
2.1 Mass Transfer Coefficients for Spherical Bubbles
- Previous.studies on mess transfer to and from sPherical ges bubbles
have been extensive, including esnalyticel and experimental,investigations.
A brief summary'of'the‘important results is given in this section. First,
e description of the pertinent enelyticel model is presented and then a
summery of-the most recent experimental findings is given.
Figure L4 ghows the model situation of & spherical bubble of radius,
, imbedded in e stationery liguid. The bubble moves with a velocity
‘fi' relative to the 1iquid. For the case of an inert gas bubble removing
& solute ges-from a liquid, the approPriate diffu51on equation is:
2
ac 3c_ 3¢ | -
u S + v 3y D —x éya ’ (5)
velocity components in the x and y directions.
where;u,rv_
C
D
local conoentration of solute gas in the liquid,
mass diffusivity for the solute gas in the liquid.
| The velocity components u and v are generally available from a solution
~of -the momentum equations, and would satisfy the bulk liquid continuity
reletion for points in the immediate V1cinity of the bubble surface
_gfur !Vr ’ : (6)
x .
where r is the redial distance from a point on the bubble surface to the
exis of symmetry. Emphasis is placed on the immediate vicinity of the
L, )/CLI
Xenon-135 Removal Effecfi:l.ven'ess, E = ‘(CL e C
_ B 1
o
o
*—l
o
o
\h
10
4
ORNL-Dwg 68-6782
o
o
N
0.
1 2.5 .. - 1 - 2 - 5 . - 100
Mass Transfer Coefficiep;, K, (£t/hr)
Fig. 3. Xenon-135 Removal Effectiveness as a Function of L1qu1d
. Phase Mass Transfer Coefficient.
i’
»
)
11
ORNL-Dwg 68-6783
fib’ Bubble Velocity
Interface
‘Bulk Liquid
cggcentr%tion Concentration,
L oa—Ax1is of Symmetry
|
Fig. 4. Coordinates for Thin Region Near Spherical Bubble Surface.
12
bubble surface because the region of important concentreation variation is
expected to be thin, and even thinner then the region of significent velo-
city veriations. Thus for such & situstion it is reasonable to represent the
velocity in~the_immediate-viginity of -the bubble surface as
u_f:us_fu;y. - (Tl
The term u, is the velocity component in the x—direction at the surface
of the sphere, possibly non-zero since the sphere is fluid, end u s is the
derivetive of the x~component of the velocity with respect to the normal
coordinate, y, and evaluated at the bubble surface.
The tengential velocity component can'bé“determined'by integrating
the continuity equation after making use of Equation (T) Thus it is
found thet
v = -g— [rluy + u's'- ¥/2)1. - (8)
"'l|l—‘
| '
In this formuletion, it is recognized that U, end U | are functions of
the position elong the bubble surface in the x-direction.
Upon use of Equetions (7) and (8) in the diffusion equation, we find
that the solute ges concentration must satisfy the relation:
' 2
! oC 139 2 oCc ., 9C
u u ——— — o ——
(B + 0 y) = -2 = [r(uy + u e Y /2)]'ay. _D.aya. (9)
Rather then proceeding with & general discussion of this equation, we now
consider two limiting cases; namely; the situation of & rigid,inferface with
us equal to zero, and secondly the case of-zerb tengentisl stress &t the
interface. The letter case certainly is relevant for gas bubdbles in a -
liquid such thet the liquid viscosity is.many‘fimes thet of the ges vis-
cosity. Thet the rigid interface situation is elso relevant constitutes
somewhet of & paradox, but it is known thet smell ges bubbles do beheve
to some extent &s rigid spheres.
Ft
Ny
"with- C, =1leatt =0, C,
13
Rigid Interface Cease.
The eppropriate modification of Equation (9) expressed. in non~
dimensionel variables ie:
! 2 2
aC _
Wyt 1a Mata¥Ni, 2 Th (10)
8 - ’
1l Y1 axl rl‘axl 2 ayl NPe- ayl2
where
t
' u
w o X _ Y o 8
xl -— rfi s Yl = rb u. Sl - _fi_ /r ?
- b b
- r_ o - C-~-C P 2.rb Ufi
= > = ’
1 rb 1l % - C Pe D
CO'= solute gas concentration in bulk liquid,
C*¥ = solute gas concentration in interface liquid.
If we now define new position varisbles end restrict our attention to
the bubble interface region, Equation (10) reduces to
ac 3201‘ |
n =32 ° | (11)
! ' ' 99
_ 1/2
where n = (rl u l) Yla
l
dé =_————-———r————— d xl.
N u :
Pe- sl . .
Equation (11) can be expressed g5 an ordinary differential equation in.
terms of e, similarity varidble,lj -n/(9¢)l/3 thus
*',dc o8 |
az”
p = 1@ p=0sett =
14
The integration of Equation (12) can be cerried out in e straightforward
way end then the result used to obtain the mass transfer rate expressed
in terms of the Sherwood number, a'rb-KL :
| - D P
P L
Ny, = - 0.6 N1/3 of(uSl 1)1/2 roax | O 13)
es reported by Baird end Hemilec, end Lochiel end Calderbenk.’>
It should be noted that the result given by Equation (13) is general.
The specific value of the mass transfer number depends on thevnature of
the relative motion between the bubble and the surrounding liquid. Table I
gives results for u at very low and large Reynolds number flow regimes
sl
- and-the final expressions for the Sherwood number for these regimes,
based on the use of Equation (13).
Mobile Interface Case
At least for bubbles heving diemeters greater than e&.few millimeters,
the surfece condition is.more,reasonably expressed a5 being one of ~
negligible tangential stress and.having‘a non-zero tengential velocity; a
mobile interface. Thus for this situation the appropriate diffusion
equation, as obtained from Equetion (9), |
2
aC . 9 C
1 1 oC 2 1
u R .= [u r.y 1 =_—-—? (lll-)
s1 9x; r, sl 71 l] 5;;- Nog ayi
where Uy is the non-dimensional tangential velocity at the bubble inter-
face‘(qsl‘= :;EL—Q. Agein, when new position variebles are. used and ve
restrict Ub/Tb. attention to the immediete,vicinity of the bubble inter-
face, Equetion (1k) is reduced to & simpler expression:
aC) 9°C;
38 902 ° - - ' : *(lS)
where c = usl ry yl;
2(usl rl)
¥, u, S
Pe “sl
_;
- TABLE I
ANALYTICAL RESULTS POR MASS TRANSFER RATES TO SINGLE GAS BUBBLES
»i ( &
Flow Regime _Interface Condition Sherwood Number References
Case I: Rigid Inteffacg
Creeping Flow u.=0-> . 1/3
L sl o gy, = 0.99 N;. 1,13
_ ’ ' . =3
Moo < 7 u'gy =5 8in 6
i‘Lam:l'har.'Boum.laty Layer u, =0
Npe »> 1 ‘u'sl (6a sin 8)/$ Ng, = 0.84 N - Np, 13 H
' § = boundary layer thickness
Case II: ‘Mobile Interface
Creeping Flow u ., _8in 6 '
' ?l 2 Bg, = 0.65 Npe 1/2 1,13
HP\e <1l u sl =0 :
Potential Flow ‘-‘,1 =3 sin 0 ' 1/2
‘ v o
Npo > 17 v 0
16
Equation (15) has a similerity solution in terms of the variable L.j
E = 0/281/2 which satisfies the ordinary differentiel equation
dacl acy - 3
—5 t 2 dg = 0 o (16)
da E \ :
with.Cl_# lat E=0 and-Cl = 0 at £ = », Lochiel and'Calderbank13
give the solution for the concentration function as: ‘
_ c H
c, = P dE. ' (17)
- | o
The concentretion gradient at the bubfile interface cen be obtained from
Equation,(17)-and the average mess transfer rate to the bubble can be
evaluated. The result in terms of the Sherwood mass trensfer number ,
=:2rbKL/D.is:
T - qi/2 o "
2 2, e
NSh - S ‘g uSl .rl dxl NPe . - (18) -
o
Table I elso includes results from the literature which deal with
the mobile interface situetion. It is important to,note;that—thé mbbile
interface results show thet the mass transfer coefficient, expréSSed as
the non—dimensional Sherwood number- (KLdb/D)’ varies with the Peclet
number (dbU /D) raised to the one-half power. In the case of the rigid
interface. bubble the Sherwood number varies with the Peclet number raised
to the one-third power. The higher power. on the,Peclet‘number giyes rise
to significantly higher mess transfer coefficients for the xenon-135,
fuel salt.systgm if the mobile interface bubble case;ié applicabie, _
The anelyticel results given in,Table I egree in general with those
obtained by other investigators. In 1935 Higbie'
contribfition to the mess trensfer literature in his,analysié of;the rete
made an importent
of ges ebsorption from bubbles rising in liquids. The enelysis was, based
on & mobile interface model and the assumption‘that the liquid surround—
ing e bubble is continuously replenished with fresh liquid as ifi rises
throfigh & liquid pool. A golution of .the time dependeht difffision equeation
L;;
17
wes .obtained which can be expressed &s:
5 1/2
‘ o 2
! Nn =17z 5o | (19)
wvhere te is the exposure time of the bubble to a given liquid envelope.
Then on the assumption that the liquid exposed to the liquis is renewed .
each.time.thatwthe bubble moves through a héight:equgl to the bubble
diemeter, equation (19) is equivelent to:
a2
Nen (20)
Thus Higbie's'result is identical to the mobile-interface equétion of
.Boussinesq.3 '
Ruckénstein;é'has elso considered mass transfer between spherical
bubbles end liquids_by solving the mess convéction equations for various
hydrodynamic situatiqns.,-In essence his development follows that pre-
sented here and the results for the extreme cases of the rigid interface
end the mobile interface agree rather well with the equations given in
Teble I. In particular Ruckenstein found
1/3
= l.Qh Npe ' ~» rigid interface, Np <1, (21)
Noy Re
and
l/?, mobile interface, N, < 1. (22)
"N, = 1.10 N Re
‘Sh - Pe
The constent in'EQnationi(22) for the mobile—interfaée bubble at low
»Reynolds numbers differs significantly frqm the corresponding equation of .
Lochiel and Calderbank.13
2s2"Egperimental'Data7on,Mass.Transfer\Coefficiénts;tc‘Single;Bubbles
Rather comprehensive surveys of the experimental dsta on mess trans—
fer coefficients for gas bubbles have been reported -in’ the litere-
tup h 5 13,1k
date from these reférenCQS‘indicate thaet gas bubbles of diemeter less than
2 millimeters behave &s rigid interface particles, and that gas bubbles
of diemeter greater than 2 to 3 millimeters seem to behave as mobile-
No attempt will ‘be made to give detailed results, however,
18 . | :
interface perticles, es shown by their fluid drag and mess transfer | kbj
characteristics. o .
- Scott and Haydule carried out pipeline contactor experiments with
verious ‘liquids using carbon dioxide end helium as solute gases. The
experimental variebles covered in the mass trensfer tests were:
Liquid superficial velocity - ~~ 0.5 to 3.6 ft/sec
Liquid phase diffusivity @ 0.1h x 10-5 to 4.8 x 10-5 cm2/sec
Gas-liquid interfacial tension 23.4 to 73.5 dynes/cm
Liquid viscosity - ‘" 0.6 to 26.5 centipoise
Tube diemeter .23 to 2.50 cm
An empirical correlation equation which described their results is:
0.0068 ¥, ¢o.7hh oo.sli'no.088D0.390'
= 4+ _
e = — - 1.88. #15%, . (23)
- mase transfer coefficient (ft/sec) £t bubble surface | |
' -t~ -contactor colume - A
t{f
<
I
‘liquid velocity in pipeline contactor, ft/sec.
liquid surface tension, dynes/cn,
liquid viscosity, centipoise,
liquid phese diffusivity, em2/sec x 107,
pipe diemeter, cm,
I
e o O r QqQ
"
volume fraction of gas bubbles in contector.
Use of the MSER heat exchanger flow dets and physical properties
of the MSER fuel selt in Equation (23) gives = 2(7 hr=1, If one
assumes & bubble surface area of 3000 £t2 (0.02 in diemeter bubbles) dis-
persed over the 83 £t3 of fuel. gystem, this result is equivalent to 8 mess
transfer coefficient of 7.7 ft/hr.
| Lamont'and Scott12 also reported experimental studies on the pipeline
contacting of .carbon dioxide bubbles end weter under cocurrent flow con-
ditions. . Experimental variables covered in the mess transfer tests were:
Liquid Reynolds numbers L 1800 - 22 hOO |
Bubble diemeter | _ , ,‘0.227f.0.55lcm
Tube diemeter - - .0.793 cm,
C
9 . M
19
An empiricel correlation equation which fits their data is:
K, = 0.030 80:"7 (228%), , (24)
where
KL = mass transfer coefficient (em/min),
NRe 1iquid phase Reynolds number, dVp/u
If one assumes & reesonable non-dimensional form consistent with
Equetion (2k4) and mekes use of the physicel properties of the carbon
dioxide-weter system, the reported correletion equation mey more properly
be written es:
d
—-K" = 1.02 Np: 49 N2, (25)
c-
vhere _
TN, = Sclrmidt number , (u/p4D)
a |
—5—-— Pipeline Sherwood number.
It is then found thet for the MSER fuel salt Equation (25) gives &
mess transfer coefficient Ei 6.1 ft/hr.
Various authors 9 20 have cited the influence of surfactants, which
sccumulate in the ges bubble interfece, on the motion of ges bubbles.
In perticuler, it is found that such interface contamination brings about .
"solidificetion" or "rigidity" of the gas-liquid interface. Under the con-
ditions of & rigid interfece due to presence of surfactants in the inter-
face bubbles, follow the welleknown"Stqkes dreg reletion
at low Reynolds numbers, vhile under conditions of & .clean interface the
bubbles show & drag behavior represented by
16
‘D LNRe
et low Reynolds numbers.
20
As pointed out earlier in this paper the "solidificetion" of the
gas bubble interface would bring about a reduction in the rate of mass.
transfer to & ges bubble interface.- Griffith 19 hes shown specific ev1—
dence of this- effect in citing the results on the reduction in solution_
rates of oxygen bubbles as surface active matter is adsorbed at the bubble -
interface. . |