JmI.IRNAI_ I:::IF" T H E ELEP.TRI-IP.

HEMII3AL SI"II IETY

OCTOBER
~----AND T ~ " ~ - ~ N ~ L . ~ ~" ,, , ~ 1

1981

Conductivity of KOH Electrolyte Supersaturated

with Zincate
Ming-Biann Liu,* Brian R. Faulds,z G. M. Cook,* and N. P. Yao*
Argonne National Laboratory, Chemical Engineering Division, Argonne, Illinois 60439

ABSTRACT
The specific conductivity of 7.32N KOH electrolyte with zincate concen-
trations ranging from 0 to 1.5M has been measured. The electrolyte conductivity
was found to decrease with increasing zincate concentration. This finding is
consistent with predictions based on the mixture rule. The equivalent con-
ductance of 7.32N potassium zincate of 7 • 5 mho 9 cm/equiv, m a y indicate
the formation of neutral associated ion pairs from potassium and zincate ions
in the electrolyte. F u r t h e r calculations indicated that the mixture rule yields
predictions of conductivities for the K F - K O H and K2COa-KOH systems that
are in good agreement with experimental data in the literature.

The p r i m a r y purpose of this study was to obtain spe-
cific conductivity data for 7N KOH electrolyte super-
saturated with zincate. These fundamental data are
needed for engineering analysis of zinc porous elec-
trodes used in alkaline batteries under development
for n e a r - t e r m use in electric vehicles. These data also
provide a baseline for the evaluation of modifications of
b a t t e r y electrolyte.
The electrolyte in Ni/Zn batteries is initially about
31% KOH (7N) saturated with ZnO. During cell dis-
charge, the concentration of zincate has been observed
to rise by three to four times the chemical solubility of
ZnO in KOH solution (1-3). Furthermore, the conduc-
tivity of the electrolyte at a given concentration and
temperature has been found to decrease linearly with
an increasing amount of dissolved ZnO up to saturation
concentration (4-6). We have determined the conduc-
tivity of the KOH electrolyte with zincate concentra-
tions up to twice chemical saturation.
During the discharge of zinc/nickel oxide cells, the
reactions for the zinc electrode may be written as fol-
lows
Zn + 4 O H - --> Zn(OH)42- + 2 e - [1]
The zincate species m a y also precipitate to form zinc
oxide according to the reaction
Zn (OH)42- -) ZnO + H~O + 2 O H - [2]
For the nickel oxide electrode, the reaction is
NiOOH(s) + H20 -{- e - ~ Ni(OH)2(s) nu O H - [3]
Thus, the net reaction of the cell system may be written
as
Zn -{- 2NiOOH(s) H- (2 -- y) H20 + (2 -- 2y) O H -
-# (I -- y) I n ( O H ) 4 ~- + 2Ni(OH)s(s) nu y Z n O ( s )
[4]
* Electrochemical Society Active Member.
Present address: D e p a r t m e n t of C h e m i s t r y , U n i v e r s i t y of Wis-
c o n s i n , Milwaukee, Wisconsin 53201.
Key words: mixture rule, K O H - K F , KOH-K2Co3.
where y is the molar fraction of zincate species precipi-
tating to form ZnO. Reaction [4] suggests that the
electrolyte is a ternary system consisting of potassium
hydroxide, potassium zincate, and water.
Ternary electrolyte theory developed from the p r i n -
ciple of irreversible thermodynamics has been de-
scribed by Miller (7) and Sunu and Bennion (8). To
predict the transport properties of a t e r n a r y electrolyte
system by using the theory, one has to estimate the
values of six solvent-fixed ionic transport coefficients.
Miller (7) s empirically that, for seven ternary
alkali halide mixtures at total concentrations ranging
from 0.5 to 3N, the ionic transport coefficients (lij) can
be closely approximated using lij data from a p p r o p r i -
ate binary systems. These estimated values of t e r n a r y
l U yield good estimates of transference numbers, con-
ductances, and solvent-fixed thermodynamic diffusion
coefficients. In our system, sufficient conductivity data
for potassium zincate are lacking. Therefore, this
theory cannot be used to analyze our conductivity data.
However, the conductance, A123, of the seven alkali
halide mixtures can also be predicted at low concen-
trations by the solution mixture rule (7), which states
that
A123 : X2A12 + X3AIs [B]
where An (i = 2, 3) is the conductance of the b i n a r y
electrolyte at the same total equivalent concentration,
N, of the mixture and where the equivalent fractions,
Xi, are given by
Nl
X i = - - i=1,2,3 [6]
N~+N8
X1 = X2 + X8 = I [7]
Substituting Eq. [7] into Eq. [5], one obtains
AI~3 = A13 -- (AI3 -- AI~)X~ [8]
In this study, we found that our conductivity data
for the KOH-K~Zn(OH)4 system and the data for the
K O H - K F system (9) and the KOH-K2CO3 system (10)
are consistent with the solution mixture rule.

2049
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 2050 J. EZectrochem. Soc.: E L E C T R O C H E M I C A L S C I E N C E A N D T E C H N O L O G Y
Experimental
F i g u r e 1 shows the s c h e m a t i c d i a g r a m of t h e e x -
p e r i m e n t a l apparatus, which consists of (i) zincate
g e n e r a t i o n cell, (ii) e l e c t r o l y t e pump, (iii) p o w e r
supply, a n d (iv) electrolyte reservoir. The Lucite
zincate g e n e r a t i o n cell was at r o o m t e m p e r a t u r e
(22~ The v o l u m e of t h e cell was about 125 ml. The
w o r k i n g electrode was an a r r a y of four zinc sticks w i t h
dimensions of 0.7 • 0.7 • 10.5 cm; these sticks w e r e
m a n u f a c t u r e d b y J. T. B a k e r Chemical C o m p a n y
(Phillipsburg, New J e r s e y ) , a n d h a d a p u r i t y of 99.6%.
To p r e v e n t the r e m o v a l of zincate f r o m the electrolyte,
a n i c k e l oxide counterelectrode, o b t a i n e d f r o m Y a r d n e y
Electric C o m p a n y (Pawcatuck, Connecticut), was used.
A p o l y p r o p y l e n e separator, p u r c h a s e d from S p e c t r u m
Medical Industries, I n c o r p o r a t e d (Los Angeles, Cali-
f o r n i a ) , was placed b e t w e e n the two electrodes to
p r e v e n t electrical shorting. A n H g / H g O r e f e r e n c e elec-
trode was used to m o n i t o r the electrode po,tentials.
A n o x y g e n - f r e e n i t r o g e n s t r e a m was i n t r o d u c e d into
the cell to e l i m i n a t e CO2 f r o m air. The electrolyte
r e s e r v o i r was a 500 m l P y r e x t h r e e - n e c k e d r o u n d -
b o t t o m e d flask w h i c h was k e p t in a constant t e m p e r a -
ture w a t e r b a t h at 25~ The electrolyte was 7.32N
K O H ( r e a g e n t g r a d e ) in d o u b l y distilled w a t e r w h i c h
was i n i t i a l l y s a t u r a t e d w i t h zinc o x i d e (0.64M) ( a n a -
l y t i c a l r e a g e n t q u a l i t y ) . No f u r t h e r purification of
these m a t e r i a l s was a t t e m p t e d . The e l e c t r o l y t e was
p r e p a r e d w i t h d o u b l y distilled w a t e r .
A t the b e g i n n i n g of the e x p e r i m e n t , the cell a n d
the r e s e r v o i r were filled w i t h the electrolyte. D u r i n g
the discharge of the cell, the e l e c t r o l y t e was c o n t i n u -
ously p u m p e d b y a p o l y p r o p y l e n e bellow pump, m a n u -
f a c t u r e d b y G o r m a n - R u p p Industries (Bellville, Ohio),
from the r e s e r v o i r to t h e b o t t o m of the cell a n d then
allowed to overflow from the top of the cell back to
the reservoir. The flow r a t e was a d j u s t e d so t h a t no
gas b u b b l e s w e r e t r a p p e d in the overflow stream.
The electrical circuit for the e x p e r i m e n t is i l l u s t r a t e d
in Fig. 1. To m a i n t a i n a constant c u r r e n t level r a n g i n g
from 0.6 to 1.2A ( a b o u t 10-20 m A / c m 2 on Zn elec-
t r o d e ) , a d u m m y resistor was placed b e t w e e n the
w o r k i n g electrode (WE) connector and the reference
electrode (RE) connector of the W e n k i n g H P 7 2 p o -
t e n t i o s t a t m a d e b y G. B a n k E l e c t r o n i k (West G e r -
m a n y ) . The p o t e n t i a l of the cell as well as t h a t of the
n i c k e l oxide electrode w i t h r e s p e c t to t h e Hg/I-IgO
r e f e r e n c e electrode w e r e r e c o r d e d on a s t r i p - c h a r t
WENKING HP72
POTENTIOSTAT
I I t "-~ ELECTRODE
- - CE1 RE ,~,.vv~.
~ - - ] = ~ 1 ~ z n ELECTRODE
RESE / MOM
~ - ~ PUMP
1 I~ ' ~ - ~ CONSTANT
TEMPERATURE
BATH
Fig. 1. Experimental apparatus
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October 1981
r e c o r d e r ( H e w l e t t - P a c k a r d 7100 BM). W h e n the r e -
c o r d e r i n d i c a t e d t h a t t h e p o t e n t i a l of t h e n i c k e l oxide
electrode h a d d r o p p e d to 0.2V vs. the H g / H g O elec-
trode, ceil discharge and e l e c t r o l y t e circulation were
stopped. The nickel oxide electrode was t h e n r e m o v e d
a n d r e c h a r g e d in fresh electrolyte in a cell using a
nickel plate as a counterelectrode. Subsequently, the
.charged n i c k e l oxide electrode was r e t u r n e d to the
zincate g e n e r a t i o n celI a n d the zincate g e n e r a t i o n p r o -
cess continued. This p r o c e d u r e was r e p e a t e d s e v e r a l
times until the desired level of zincate concentration
was obtained.
A f t e r completion of each discharge, time was allowed
for the e l e c t r o l y t e in the r e s e r v o i r to r e t u r n to 25~
Next, 1 ml aliquots of this e l e c t r o l y t e were p i p e t t e d
for the d e t e r m i n a t i o n of zincate concentration b y t i t r a -
tion w i t h 0.1M E D T A ( e t h y l e n e d i a m i n e t e t r a a c e t i c acid)
w i t h E r i c h r o m e Black T as an indicator. The specific
c o n d u c t i v i t y of the e l e c t r o l y t e in the r e s e r v o i r was
m e a s u r e d at different zincate concentrations (0-1.52M),
using two conductivity cells in conjunction w i t h an
a - c conductivity b r i d g e o p e r a t e d a t a f r e q u e n c y of
1 kHz. The conductivity cells w e r e Models G50 and
G100 Beckman Instruments, I n c o r p o r a t e d ( C e d a r
Grove, New J e r s e y ) ; the conductivity b r i d g e was
Model 3I, Yellow S p r i n g s I n s t r u m e n t Company, I n -
c o r p o r a t e d (Yellow Springs, Ohio). The cell constants
w e r e c a l i b r a t e d using 0.1N KC1 (specific c o n d u c t i v i t y
0.11134 m b o / c m ) (11) and f o u n d to be 50.899 c m - 1 for
the Model G50 and 99.857 cm -1 for the Model G100. To
m a k e the c o n d u c t i v i t y measurement, the e l e c t r o l y t e
was sucked into the c o n d u c t i v i t y cell a n d a conductance
r e a d i n g completed w i t h i n 30 sec. I n this m a n n e r the
change in t e m p e r a t u r e is minimal.
W h e n the concentration of zincate was above 1.3M,
w h i t e p r e c i p i t a t e was o b s e r v e d in the electrolyte.
Therefore, s e v e r a l hours w e r e allowed for the p r e -
cipitate to settle to the b o t t o m of the reservoir. P o r -
tions of clear e l e c t r o l y t e were t a k e n for the d e t e r m i n a -
tion of specific c o n d u c t i v i t y and zincate concentration;
there w e r e at least two m e a s u r e m e n t s m a d e for each
determination. F o r one determination, e l e c t r o l y t e t a k e n
from t h e r e s e r v o i r was v a c u u m filtered t h r o u g h 0.2
~m filter paper. The result of this m e a s u r e m e n t was
in a g r e e m e n t w i t h those o b t a i n e d using clear unfiltered
electrolyte. The a v e r a g e u n c e r t a i n t y for a l l the m e a -
s u r e m e n t s was 1.5 %.
Results and Discussion
The specific c o n d u c t i v i t y d a t a a l o n g w i t h d a t a o b -
t a i n e d from other studies (5, 6, 9) u n d e r s i m i l a r con-
ditions are p r e s e n t e d in g r a p h i c a l form in Fig. 2. This
figure shows t h a t a least squares fit of our specific
conductivity d a t a is in .agreement w i t h those of the
I I I
0.6 (
E
F-
0.4
(D
C~
Z A DIRKSE, 7.4 N KOH, 25~
O
0.2_ - - 0 BAKER AND T R A C H T E N B E R G , 6.9 N KOH, 25~ __
(D
U_
[] THORNTON AND CARLSON, 7.1 N KOH~ 26.4~
0 THIS WORK, 7.52 N KOH, 25%
UJ
D_
r
o I I t
0.5 1.0 1.5 ~-.0
ZINCATE CONCENTRATION, M
Fig. 2. Specific conductivity of KOH electrolytes as a function of
zincate concentration.
 V o L 128, No. 10 CONDUCTIVITY OF KOH ELECTROLYTE 2051

other workers. This figure also indicates t h a t the
conductance of the e l e c t r o l y t e m a y be l i n e a r l y c o r r e -
lated w i t h zincate concentration. A l i n e a r r e l a t i o n s h i p
for conductivity vs. weight p e r c e n t of ZnO was also
o b s e r v e d b y Dyson et al. (4) up to chemical s a t u r a t i o n
of ZnO in more concentrated K O H e l e c t r o l y t e (namely,
35-46% b y w e i g h t or 8.3-11.6N). The l i n e a r r e l a t i o n -
ship shown in Fig. 2, b e t w e e n the specific conductivity,
k, and the m o ! a r concentration of zincate, Czn(n), can
be e x p r e s s e d b y the equation
of p o t a s s i u m ions p e r 2 e - w e r e t a k e n up from the
charging cell and r e l e a s e d in the zincate g e n e r a t i n g
cell. F o r our m a x i m u m zincate concentration of 1.53M,
the concentration of potassium ions is e s t i m a t e d to
increase b y a m a x i m u m of 0.15N or 2% of its original
value. Therefore, we m a y assume that the concentra-
tion of potassium ions in t h e e l e c t r o l y t e t h r o u g h o u t
the e x p e r i m e n t did not change. W h e n d i v i d e d b y the
total e q u i v a l e n t concentration (7.32N), Eq. [9] is
t r a n s f o r m e d to

k ---- (0.637 _+ 0.011) -- (0.159 __ 0.009)Czn(n) m h o / c m A~23 = (87 _+ 2) -- (80 __ 5) X2 mho 9 cm~/equiv. [10]

[9] w h e r e subscripts 1, 2, a n d 3 designate potassium,

The slope of 0.16 for this equation is higher t h a n the
slopes e s t i m a t e d f r o m the d a t a a t 25~ given b y Dyson
et al. (4) (slope of 0.13 for 35% KOH, 0.11 for 40%
KOH, 0.095 for 46% K O H ) . These values i n d i c a t e d
t h a t the specific zincate conductance decreases w i t h
increasing K O H concentration. We also found that
the specific c o n d u c t i v i t y of K O H decreases w i t h i n -
creasing K O H concentration (k -- 0.64 m h o / c m at
31% KOH, 0.58 m h o / c m at 40% KOH, and 0.45 m h o /
cm at 46% K O H ) (4).
The zincate species in the solution of ZnO in K O H
is Z n ( O H ) 4 2 - as evidenced b y n u c l e a r m a g n e t i c
resonance (NMR), Raman, a n d i n f r a r e d reflection
spectroscopic studies (12-14). I n the s u p e r s a t u r a t e d
solution, Dirkse (12) i n d i c a t e d t h a t the zincate species
is also Z n ( O H ) r 2-. However, Briggs et al. (1) con-
cluded from t h e i r spectroscopic s t u d y that the zincate
species in the s u p e r s a t u r a t e d state is i n i t i a l l y Zn{OH)42-
and s e q u e n t i a l l y b e c o m e s . [ Z n ( O H ) 3 ( H 2 0 ) ] - and
[Zn (OH) 2 (H20) 2] as the degree of s u p e r s a t u r a t i o n i n -
creases. If there were a n y species other t h a n Zn(OH)42-
in our e x p e r i m e n t , a change in the slope of the plot in
Fig. 1 w o u l d have b e e n detected as was shown in the
plots of emf vs. l o g ~ 0 { [ Z n ( I I ) ] / [ O H - ] 4} given b y
Briggs et al. (1). We find no such evidence in Fig. 1.
Therefore, we conclude that the zincate species in the
s u p e r s a t u r a t e d solution is the same as t h a t in the
solution of ZnO in KOH. Therefore, Eq. [1] is the
electrode reaction.
According to Eq. [6]-[8], the c o n c e n t r a t i o n of po-
tassium ions is r e q u i r e d to a p p l y the m i x t u r e rule to
our data. The initial concentration of potassium ions
was 7.32N. This value m a y be changed in the dissolu-
tion of ZnO and Zn due to possible change in the elec-
t r o l y t e volume a n d t a k e - u p / r e l e a s e of potassium ions
b y the n i c k e l oxide electrode. W e i n v e s t i g a t e d these
two possible ways for changing the K + concentration
and found the change to be n e g l i g i b l y small. In the
chemical dissolution of ZnO and anodic dissolution of
Zn, the change in the e l e c t r o l y t e volume is small. This
is justified b y the fact t h a t the a d d i t i v e rule predicts
values w i t h i n 1% of the d e n s i t y d a t a given b y Dirkse
(5) for the solution of ZnO in K O H electrolytes and
values w i t h i n 3% of the d e n s i t y d a t a given b y Eisen-
berg et al. (15) for s u p e r s a t u r a t e d zincate solutions.
E x p e r i m e n t a l evidences (16, 17) indicate t h a t p o t a s -
zincate, and h y d r o x i d e ions, respectively. Thus, f r o m
Eq. [8], it can be concluded that A18 ---- 87 _+ 2 m h o .
cm2/equiv, and Az3 -- A~2 = 80 ___ 5 mho 9 cm2/equiv.
In other words, the a p p a r e n t e q u i v a l e n t conductances
are 87 _-+_-2 mho 9 cm2/equiv, for p o t a s s i u m h y d r o x i d e
and 7 _+ 5 m h o . cm2/equiv, for potassium zincate in
the electrolyte. W h e n the m i x t u r e rule is a p p l i e d to
the clata given b y Dyson et al. (4), values of a b o u t
zero are also obtained for the conductance of potassium
zincate. This low value of e q u i v a l e n t conductance for
potassium zincate indicates that p o t a s s i u m ions a n d
zincate ions are l i k e l y to form n e u t r a l associated ion
pairs in the electrolyte.
If the m i x t u r e rule is a v a l i d a p p r o x i m a t i o n for con-
c e n t r a t e d solutions, then it can be used to e s t i m a t e the
conductance of t e r n a r y electrolyte systems f r o m the
a v a i l a b l e conductance d a t a of b i n a r y e l e c t r o l y t e sys-
tems (19). Conductivity d a t a of the K O H - K F system
(9) (7.13 ___ 0.16N), the KOH-K2CO3 s y s t e m (10)
(8.35 _+ 0.23N), and o u r K O H - K 2 Z n ( O H ) 4 system.
(7.32N) are plotted in Fig. 3 as a function of e q u i v a l e n t
fraction. It should be noted t h a t t h e r e was a p r o b l e m
with Ref. (10). The d a t a in Ref. (10) w e r e given in
both g r a p h i c a l and t a b u l a r forms, which was not con-
sistent. It was decided to select t h a t set of d a t a for
which the K O H values w e r e consistent w i t h those c a l -
culated f r o m the table given in Ref. (19). Results of
least squares analyses of these d a t a a r e shown in Fig.
3 and Table I. As can be deduced for each e l e c t r o l y t e
system in Table I, the conductance d a t a of the b i n a r y
system are in good a g r e e m e n t with those for the t e r -
n a r y system; the m a x i m u m difference b e t w e e n the e x -
p e r i m e n t a l d a t a and the t e r n a r y system d a t a ( o b t a i n e d
from analyses of b i n a r y d a t a using m i x t u r e r u l e )
shown in Fig. 3 is six e q u i v a l e n t conductance units for
the K O H - K F system and five e q u i v a l e n t conductance
units for the KOI-I-K2CO3 system.
EQUIVALENT FRACTION, x 2
KOH KF
.> 0.4 0.8
I I I I '
&o~ ' I '
N 7.15 N KOH-KF
E A=(114 +1) - (55-+ 2)x 2
o 25~
oI /h=(90+4)-(45+5)x 2
120 l
E / 7 . 5 2 N KOH-K2Zn(OH) 4
/25 ~ C

~
G
sium ions a r e t a k e n up b y nickel o x i d e electrodes d u r - 0 80+5)x z
ing ~he .charge cycle, and r e l e a s e d d u r i n g the discharge 801
cycle. A r e c e n t s t u d y b y B a r n a r d et al. (17), indicates
O
that the t a k e - u p / r e l e a s e of potassium ions depends on Z 0~.
0
o
the crystal s t r u c t u r e of the nickel oxide electrode: 40
0.102 tool p e r 2 e - for fl-NiOOH and 0.47 mol p e r 2 e - Z
for ~-NiOOH. H a r i v e l et al. (18) indicated t h a t the ILl
--I
.h=(69 + 2)-141+4)x 2
f o r m a t i o n of fl- and %,-NiOOH depends upon the c h a r g -
ing rate, the state of charge, a n d the e l e c t r o l y t e con- o , I , r , ', I , [ J
0 0.4 0.8 0 0.4 0.8
centration. In our study, the n i c k e l oxide electrode
KOH K2Zn(OH) 4 KOH K2CO3
was c h a r g e d at 6 m A / c m 2 up to 20% of t h e o r e t i c a l
c a p a c i t y (3 A - h r ) in a cell with fresh electrolyte and EQUIVALENT FRACTION, x 2
then discharged in the zincate g e n e r a t i n g cell. U n d e r Fig. 3. Equivalent conductances of KOH-K2Zn(OH)4 system,
such conditions, o n l y fl-phase m a t e r i a l s a r e e x p e c t e d KOH-KF system and KOH-K2CO.~ system as a function of equiva-
to be formed. Therefore, we estimate t h a t 0.102 mol lent fraction.

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 2052 J. EIectrochem. S;oc.: ELECTROCHEMICAL SCIENCE AND TECHNOLOGY October 1981

Table I. Values of A13 and -~la -- A12 obtained from binary system data and least squares
analyses of ternary system data using the mixture rule (Eq. [8])

Binary system data,~ Ternary system data,b

rnho 9cm2/equiv, mho 9cm2/equiv.
Concen. Temper-
Electrolyte tration, N ature, ~ A~ A~ A18 -- A~ A~ als -- a ~

KF-KOH 7.13 25 43 89 46 90 -- 4 45 -----5

IGCO~-KOH 8.35 20 30 70 40 69 ~ 2 41 ~ 4
K~CO~-KOH 8.35 40 44 96 52 94 ----.2 52 -----3
K~CO~-KOH 8.35 60 59 113 54 114 __. 1 55 • 2
IGZn (OH),-KOH 7.32 25 -- 88 -- 87 • 2 80 -----5

9Obtained from Ref. (9) and (10) and this work except for the v a l u e o f An f o r KF, which was calculated from the table given in
Ref. (12).
Ref. (9) and (10) [see text for a discussion of the data from R~f. (10)].
b C a l c u l a t c d f r o m o u r data and t h o s e f r o m

Summary
1. The specific conductivity of 7.32N KOH electrolyte
at different zincate concentrations was measured. The
conductivity of the electrolyte was found to decrease
linearly with increasing zincate concentration. This is
consistent with predictions based on the solution mix-
ture rule (7).
2. A least squares analysis of our data by using the
mixture rule indicates that the equivalent conductances
of potassium hydroxide and potassium zincate (7.32N)
at 25~ are 87 • 2 and 7 • 5 mho 9cm2/equiv., respec-
tively. This low value of equivalent conductance for
potassium zincate indicates that the potassium and
zincate ions are likely to form neutral associated ion
pairs in the electrolyte.
Acknowledgments
This work was supported by the U.S. Department of
Energy, Division of Electrochemical Energy Storage
Systems. We thank Yardney Electric Company for pro-
riding nickel oxide electrodes.
Manuscript submitted Jan. 28, 1981; revised manu-
script received March 25, 1981.
Any discussion of this paper will appear in a Discus-
sion Section to be published in the June 1982 JOUa~AL.
All discussions for the June 1982 Discussion Section
should be submitted by Feb. 1, 1982.
Publication costs o~ this article were assisted by Ar-
gonne National Laboratory.
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