CHAPTER1:

THERMODYNAMICS
O F E L E C T R O LY T E S
Trần Thụy Tuyết Mai, PhD.
Email:[email protected]

Division of Physical Chemistry – Faculty of Chemical Engineering

HCMC University of Technology - VNU-HCM 1
 CONTENTS
1. Introduction

2. Thermodynamic properties

3. Debye-Huckel limiting law

4. Electrical conductivity

5. Transport number

[1] P.W.Atkins, “Physical Chemistry”, Oxford University press, 2004.

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 INTRODUCTION OF
ELECTROLYTES

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 A Sugar Solution

NaCl(aq.)  sodium chloride solution HC2H3O2(aq.)  acetic acid solution

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 WHAT IS ELECTROLYTE
• Electrolyte: is a chemical compound which produces ions when dissolved in a
polar solution such as H2O (dissociates into ions). These ions have either a
positive or negative electrical charge, which is why we refer to these compounds
as electro-lytes.

• An electrolyte is an
electric conductor; unlike
metals the flow of charge is
not a flow of electrons, but
is a movement of ions.

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 ELECTROLYTE SOLUTIONS

 Homogeneous
 Compositions can vary in a range
 Can allow the electricity current to pass
through by the electron transport by ions in
the solutions

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 MOLTEN SALT
https://www.youtube.com/watch?v=NafNIn4R8tg4

The salt in its solid state or in the

crystal structure are fixed in a 3D
lattice, the ions are bound together
by very strong ionic bonds, and not
broken easily. So in solid salt, there
are no free ions, they are fixed in the
lattice structure.
For Molten salt, this ionic bonds are
broken, and thus ions are free to
move and more mobile  presence
of free ions.
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 ELECTRO- ELECTROLYTE
DISSOCIATION SOLUTION

Vapor Pressure Lowering

Dissociation of electrolyte is a process & Osmotic Pressure
that breaks electrolytes into ions in Freezing Point Depression &
polar solvent or that melts ionic Boiling Point Elevation
compounds to generate ion flows
Electrical conductor

Electrolyte: is a chemical compound that is dissociated

into ions (partially or totally) in polar solutions or under a
melting process at high temp. to generate ion flows
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 ELECTRO- DISSOCIATION (DISSOCIATION)
A+B-  +Az+ + -Bz-
Dissociation constant KD
 
( n ) .( n ) n: mol, ion-mol concentration
KD 
n A B
 

The percent ionization of a solution (% Ion)  of dissociated molecules

The percent dissociation   of the total dissolved molecules

Strong Non Weak

electrolyte electrolyte electrolyte
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10

DISSOCIATION
• Strong electrolyte: dissociate totally
HCl(aq)  H+(aq) + Cl-(aq) • Weak electrolyte: dissociate partially

CH 3COOH( aq)  CH 3COO  ( aq)  H  ( aq)

Equilibrium
 2C
constant KC 
1 Initial
concentration
of acetic acid

KC

C
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 DISSOCIATION

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 VAN’T HOFF FACTOR
The van’t Hoff factor (i): the ratio
of moles of particles in solution to
moles of formula units dissolved.

 = imRT (osmotic pressure)

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 Mg(NO3)2(aq)  Mg2+(aq) + 2NO3-(aq)
DISSOCIATION
Increasing the
A+B-  +Az+ + -Bz- number of particles
in solution
(n0  n0 .)    .n0 .    .n0 .
i
n0
with :  = + + -
i 1
i = 1 + (-1). 
 1
• Dilute solutions: i  14
• Weak electrolytes: small  ,  0; i  1
• Strong electrolytes:   1 ; i = 
[email protected] – Ex: Inorganic soluble salts, acids, bases
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 The freezing point of an aqueous 0.050 m CaCl2 solution is -0.27
0C.What is the van’t Hoff factor (i) for CaCl at this concentration?
2
How does it compare to the expected value of i ?

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 EFFECT OF SOLVENT ON IONIC DISSOCIATION

H2O Ethanol H2O + Ethanol

• HCl (gas) / solvents of
benzene; hexane  non-electrical • CH3COOH / aqua ammonia 
CH3COOH dissociates completely,

LiCl is a strong electrolyte in water

but a weak electrolyte in propanone. The percent dissociation depends
on the nature of solvent
(permittivity of the medium: )
[4] http://chemistry.tutorvista.com/inorganic-chemistry/proton-donor.html
[email protected] [5] http://www.verticallearning.org/curriculum/science/gr7/student/unit01/page29.html 15
 THE RELATIVE PERMITTIVITY
OF THE MEDIUM
• The relative permittivity can have a very significant effect on the
strength of the interactions between ions in solution.

• Relative permittivity of the medium (the dielectric constant- D or r)

0 = 8.8542*10-12 (J.coulomb/m) (F/m): the permittivity of vacuum

: the permittivity of the medium

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 THE RELATIVE PERMITTIVITY

Solvent Temp. Dielectric @ 20 0C

(oC) constant
(D)

Water 0 88
20 80.1
100 55.3
200 34.5
The relative permittivity of a substance is large if its
molecules are polar or highly polarizable.

[email protected] [3] P.W.Atkins, “Physical Chemistry”, Oxford University press, 2004

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 STATIC ELECTRICAL FORCE
BETWEEN 2 IONS
q1.q2
Static electrical force f  (Coulomb law)
4. . .r 2

(Static electric forces - Electrostatic forces- are

attractive or repulsive forces between particles
that are caused by their electric charges)

• q1, q2: charge of opposite ions

• Note: The interaction (physical/chemical) between the solvent

and the electrolyte may exist.
 SOLVATION/ HYDRATION

 Interaction solvent – ions to form relatively stable complex (solvation).

Solvent: H2O  hydration

 Number of water molecules in the complex: ligand.

 For aqua solutions of alkaline/ alkaline earth ions: formed by the ionic-
dipoles interactions which depend on: Ion electrical charges, ion radius,
and ion weight.
 SOLVATION/ HYDRATION

Kinetic diameter  270 pm

 SOLVATION/ HYDRATION

 Near hydration layer: coordination bond

(donor – accepter bond): relatively stable.

 Far hydration layer: weak static electrical

force: relatively unstable.

Solvation/ hydration
release energy
destruct crystalline solid
(break chemical bonds)
Ion Unhydrated Hydrated
radius (pm) radius (pm)
Na+ 117 358
K+ 149 331
NH4+ 148 331
Ca2+ 100 412
Mg2+ 72 428
Al3+ 53 480 Kinetic diameter  270 pm
Cl- 164 332
OH- 133 300
NO3- 179 340

Source (Volkov, A. G., S. Paula, and D. W. Deamer (1997))

 Classification of electrolytes
1. Strong/ weak / non electrolytes: depend on “”.
2. True/ potential electrolytes: depend on the nature of chemical
bonds in the molecules/ crystals

– True electrolytes: Ionic bond

– ex: NaCl, KCl, CuSO4,…
– Potential electrolytes: other bonds:
– ex: HCl, CH3COOH,
 Classification of solvents

Non- polar Polar

polar aprotic protic
solvents solvents solvents

Increase polarity
- Protic solvents: H+ donor, form hydrogen- bond between solvent
– solute (electrolytes)  can dissolve/ dissociate/ solvate to form ions
( H2O, ethanol, buthanol,…)
- Aprotic solvents: have common e- pairs  can solvate cation to
form ionic solutions (Acetone, Acetonitrile,..)
 OSMOSIS
Osmosis is the flow of solvent from a solution of lower solute concentration to one of higher solute
concentration. Concentrated solutions draw solvent from more dilute solutions because of nature’s
tendency to mix.
A semipermeable membrane —a membrane that selectively allows some substances to pass through but
not others separates the two halves of the cell. Water flows by osmosis from the pure-water side of the cell through
the semipermeable membrane and into the saltwater side.

 = imRT

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 Reverse osmosis (RO)
Water Purification system

Ion Radius
(pm)
Na+ 117
K+ 149
NH4+ 148
Ca2+ 100
Mg2+ 72
Al3+ 53
Cl- 164
OH- 133
Reverse osmosis (RO): a process by which a solvent
passes through a porous membrane in the direction NO3- 179
opposite to that for natural osmosis when subjected to a H2O 135
hydrostatic pressure greater than the osmotic pressure.

https://www.youtube.com/watch?v=ron94T_5kmA
 Water purification
Desalination
Reverse osmosis (RO) membrane pore-size ??

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2. Thermodynamic properties
 CHEMICAL POTENTIAL OF IONS

Chemical potential  (mu): the 𝐺

i =
Gibbs free energy per molar unit 𝑛𝑖 𝑗𝑖 , 𝑃 , 𝑇

Chemical energy i presents how much Gibbs free energy

changes (by dGi) if adding or removing a number dni
particles of species i in the solution while keeping the
number of other particles, P and T constant.

• + = +0 + RT.lna+
= +0 + RT.lnm+ + RT.ln+

ai = iCi
• - = -0 + RT.lna-
= -0 + RT.lnm- + RT.ln-
 Mean of concentrations & activity coefficients

M+A- +Mz+ + -Az-  /nu/: stoichiometry

z+, : z+ : oxidation state of cation & anion

m = (m++.m--)1/ m = (m++. m--)1/ Molarity

x = (x++.x--)1/ x = (x++. x--)1/ Mole fraction
c = (c++.c--)1/ c = (c++. c--)1/ Mole concentration

Relations:
m c
x  
m  1000 / M 1 c  (1000   M 2 .c) / M 1
m.M 1  c( M 1  M 2 )
ln  x   ln  m   ln(1  )  ln  c   ln(  )
1000 0 1000 0
 , 0 : density of solution, solvent (g/ml)
 ACTIVITY & RELATIVE EXPRESSIONS

Ideal solution AmBn  mAz+ + nBz-

 = 0 + RTlnC
Chemical
Strong
potential Real solution electrolytes
= 0 + RTlna = 0 + RTln.C

Activity Activitive coefficent

mz+ = nz-
Anion chemical potential: - = o- + RTln(a- )  = m+ + n-
Cation chemical potential: + = o+ + RTln(a+) o = mo+ + no-
a+ = +.C+ = m. +.C
Activity of the solute (a)
a- = -.C- = n. -.C could be measured by
a  (m n )(  )C
m n m

n

m n
experimental works
a = (a+m.a-n)1/
  mn
 = (+ m. - n)1/

a   a 1 /    C      C a = a+m.a-n = a
C = (C+m.C-n)1/
 = (mm.nn)1/
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 RESIDUAL CHEMICAL-POTENTIAL

 - id = .RT.ln

Reason: Difference in interaction of ion – ion, ion – solvent,

solvent – solvent

Significance of : the deviation of real solutions and the ideal solutions

*Very diluted solutions  Differences are not significant

  = 1
DETERMINATION OF   BY

EXPERIMENTAL METHODS

(READ TEXTBOOK)
 IONIC STRENGTH (I)

• Ionic strength of an ionic solution:

Im = 1/2.(mi.Zi2) AmBn  mAz+ + nBz-

• For solutions which consist 02 ions (01 anion, 01 cation):

Im =1/2(m+.Z+2 + m-.Z-2)
IC = 1/2.(Ci.Zi2)

mi: molarity (moles of ion/1kg of solvent)

Ci: the molar concentration (moles of ion/ 1 liter of solution)
 What happen to I ?

Im = 1/2.(mi.Zi2)

•Increase ion concentrations?

•Increase ion charges?
 Ionic strength (I)
LEWIS-RANDALL EMPIRICAL LAW

The mean ionic activity coefficients of a strong electrolyte is similar for

all solute solutions which have the same ionic strength.

For solution of a strong electrolyte,  depends on ion

concentrations and ion charges (not the nature of ions).
3. Debye-Huckel limiting law
 DEBYE-HUCKEL LIMITING LAW
(FOR VERY LOW CONCENTRATION)

Ideal solution:
 zi e 2 
2

 = o + RTlnC RT ln  i 
a = .C 3
Residual chemical potential
Real solution:
ln  i   z i2 A I
 = o + RTlna

ln     z  z  A I
In aqueous solution, 1 atm
T(oC) 0 18 25 100 Constant, f(T, P)
A 0.486 0.499 0.509 0.568

Ionic strength:
𝟏 Ci (ion-mole
I = (CiZi2) concentration) lg    0.509. Z  Z  I
𝟐
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 Extended Debye-Huckel equation
For H2O solvent at 25oC:
𝟐
−𝟎.𝟓𝟎𝟗 𝒁𝒊𝑰 (I  0.1)
lg i=
𝟏+ 𝟑.𝟐𝟗𝒂 𝑰
(Second equation)
a (nm): radius of the hydrated ion

−𝟎.𝟓𝟎𝟗 𝒁𝟐𝒊 𝑰
lg i= + 𝒄. 𝑰 (I  0.5)
𝟏+ 𝟑.𝟐𝟗𝒂 𝑰
c: experimental constant (Third equation)
Activity coefficient of ion in aqua solutions: i

lg  i   A.Z . I C
i
2

For H2O solvent at 25oC:

lg  i  0.509.Z . I C
i
2

• Limitation of the D-H law:

Correct for dilute aqua solutions (C  0.01M; I= 0.01-0.03)
and 1-1 electrolytes   = 
 i
 Ion Hydrated
radius (pm) (a)
a= 9Å, Z=1 Na+ 358
K+ 331
a= 3Å, Z=1 NH4+ 331
Ca2+ 412
Mg2+ 428
Al3+ 480
Cl- 332
OH- 300
NO3- 340

H3O+  900

a= 3Å, Z=3
 Mean of ionic activity coefficients: 

M  A     M z    A z
 = (++.--)1/ .lg = +lg+ + -lg-
= + + -
  Z 2   Z 2
lg     A IC

Because:  + .Z+  =  - Z- 
(see more in textbook)
lg     Z  Z  A I C   Z  Z  A' I m
( A'  A 0 )
For H2O solvent at 25oC : A  A’ = 0.509 (mol/l)-0.5
 Mean of ionic activity coefficients: 

lg     Z  Z  A I C   Z  Z  A' I m

For H2O solvent at 25oC: lg    0.509. Z  Z  I

C (mol/l) NaCl ZnSO4

   
(calculated) (Experimental) (calculated) (Experimental)

0.001 0.954 0.965 0.812 0.700

0.002 0.946 0.952 0.812 0.700

0.01 0.840 0.906 0.517 0.387

 Mean of ionic activity coefficients: 

Davies empirical equation:

( I 0.5 )
IC
lg     Z  Z  A  0,1( Z  Z  ) I C
1  IC

(For estimation of  )
 Applications

• Equilibrium constants
• pH calculation
• Ionic activity coefficient in solutions containing many ions
 1. Calculate the ionic strength and the mean activity coefficient of
1.00 mmol kg-1 KCl(aq.) at 25°C
2. Calculate the ionic strength and the mean activity coefficient of
1.00 mmol kg-1 CaCl2(aq.) at 25°C
3. Calculate the mean activity coefficient of 3.00 mmol kg-1 CaCl2(aq.) at 25°C, and comparing
to that of 1.00 mmol kg-1 CaCl2(aq.) at 25°C.
4. Calculate the ionic strength and the mean activity coefficient of
solution of 1.00 mmol kg-1 CaCl2(aq.) and 0.1 mmol.kg-1 NaCl, at 25°C

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 4. ELECTRICAL CONDUCTIVITY

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• Conductor: in physics and electrical engineering, a conductor is
an object or type of material that allows the flow of charge (electrical
current) in one or more directions

Electrical conductance:
the conductivities of
electrolyte solution

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 ELECTRICAL CONDUCTORS
• Type 1 (metals, semi-conductors): electrical conduction by electrons and holes
• Type 2 (electrolyte solutions, molten electrolytes) : electrical conduction by ions

Electrolysis

Conductor ion (+) Conductor

Type 1 q cation q
Type 1

ANODE ion(-) CATODE

(Oxidation) anion Reduction

2Cl-  Cl2 + 2e Conductor Cu2+ + 2e  Cu

Fe2+  Fe3+ + e Type 2 2H2O + 2e  H2 + 2OH-
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ELECTRICAL CONDUCTIVITY OF SOLUTION ()
• Conductivity (specific conductance, electrical
conductivity) of an electrolyte solution [ (-
1.cm-1 = S/cm)] is a measure of its ability to

conduct electricity.

• is measured by determining the

resistance of the solution between two flat or
cylindrical electrodes separated by a fixed
distance. The resistance is measured by
a conductivity meter.  (-1.cm-1)
at 180C
Ag 615000

 
l 1 type 1>> type 2 Solution of KCl
0.0098
 R.S >>  non-electrolyte
(1N)
Paraffin 10-18
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 CONDUCTANCE (G)
& MOLAR CONDUCTIVITY
• The conductance, G, of a solution is the inverse of its resistance R: G = 1/R. As
resistance is expressed in ohms, Ω, the conductance of a sample is expressed in Ω-1.
The reciprocal ohm used to be called the mho, but its official designation is now the
siemens, S, and 1 S = 1 Ω-1 = 1 C V-1 s-1. The conductance of a sample decreases
with its length l and increases with its cross-sectional area A (m2).
 [ S.m-1] is the conductivity
 [m]: length of conductance sample
C [mol/l]: the molar concentration of the added electrolyte
m [S m2 mol-1]: the molar conductivity
1 mS = 10-3 S

The conductivity of a solution depends on

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the number of ions present. 51
 The conductivity of a solution depends on
the number of ions present.

• the number of ions in the solution might not

be proportional to the electrolyte
concentration

• ions interact strongly with one another, the

The concentration dependence of conductivity of a solution is not exactly
the molar conductivities of (a) a typical
strong electrolyte (aqueous potassium proportional to the number of ions present.
chloride) and (b) a typical weak electrolyte
(aqueous acetic acid)

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  = F(C)
 (S/cm)
Strong electrolytes:
• Low conc. range : vion  C,  increases with
increasing C ( : proportional with ion num.)
• High conc. range : “Ion cloud”  velocity of
transportation of ions decrease  decreases

Weak electrolytes:
• Low conc. Range: low density of “ ion cloud,
vion  C, insignificant effect on 
• Increasing conc.  the percent dissociation
 
KC
  .
C
C (mol/l)
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  = (T)
T = 25 [1- (T-25) + (T-25)2]
Empirical equation:  = 0.0163 (- 0.0174)

T , 25 : electrical conductivity @ T 0C và 250C

, : constants (depend on electrolyte solutions)

Strong Strong Salt

Acid base
 0.0164 0.0190 0.022

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 EQUIVALENT CONDUCTIVITY ()

Equivalent conductivity : Conductivity

of a volume containing 1 equivalent (molar
equivalent) between 02 flat parallel same-
area electrodes with a cm distance.

1000.
 -1.cm2.eq-1
C
C: equivalent concentration (eq./l)
The concentration dependence of the molar
conductivities of (a) a typical strong electrolyte
(aqueous potassium chloride) and (b) a typical
weak electrolyte (aqueous acetic acid).
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 STRONG ELECTROLYTE SOLUTIONS
(KOHLRAUSCH’S LAW)
m°

    a C  o  a C
The constant m° is the limiting molar
conductivity, the molar conductivity in the limit of
zero concentration (when the ions are effectively
infinitely far apart and do not interact with one
another).
The constant 
(or a) is found to depend more on
the stoichiometry of the electrolyte (that is,
whether it is of the form MA, or M2A, etc.) than on
its specific identity.

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Electrolytes  Electrolyt  Difference
Kohlrausch’s law
(-1cm2mol-1) es (-1cm2mol-1)

KCl 149,9 NaCl 126,5 23,4 The limiting molar conductivity of the cations
is denoted + and that of the anions  ,
KI 150,3 NaI 126,9 23,4
then his law of the independent migration
1/2K2SO4 153,5 1/2Na2SO4 130,1 23,4 of ions states that.

At very low concentration (in the limit of zero

concentration), ions migrate independently in
solution. Meanly, no interionic interactions
is at the limiting concentration of solution

Calculating a limiting molar conductivity of BaCl2 solution at 298 K

° (12.72 2 x 7.63) mS.m2.mol-127.98 mS. m2 mol-1
m

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 WEAK ELECTROLYTES

 C 2
1 C
The percent  
K   1 dissociation 
1  K
  C
 
   K
1 1 C
 
   2 K
Ostwald’s dilution law

The graph used to determine the limiting value

of the molar conductivity of a solution by
extrapolation to zero concentration
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 TRANSPORT VELOCITY OF IONS &
ELECTRICAL CONDUCTANCE
• Symbols:  (upsilon) Stocks Equation
+ , - : transport velocity of cation, anion (cm/s) Z .eo E
(depend on nature of ion, concentration, temperature,  .
viscosity, intensity of electrical field) 6. .r. l
0+ , 0- : Absolute velocity of cation, anion (cm2.s-1.V-1)
(mobility???)
+ = 0+.(E/l) ;  - = 0-.(E/l)
[E/l: intensity of electrical field]
C,  : Equivalent concentration (eq/l), percent dissociation
C. /1000 (eq/cm3) : equivalent of cation, anion in 1cm3

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 TRANSPORT VELOCITY OF IONS &
ELECTRICAL CONDUCTANCE
• Equivalent of cation, anion transport
through area S (cm2) for 1s:
• Total quantity of electricity (I) transported by cations, anions
through S of area (cm2) for 1s:
(   ).S . .C.F (0  0 ).S . .C.F .E
I  I  I  
1000 1000l
• Ohm’s law: E E. .S E..S .C
I  
R l 1000l
• Hence,
 = .F.(0+ + 0-) (F: Faraday’s const.)
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 MOBILITY & MOLAR CONDUCTIVITY
The solution itself in the limit of zero concentration (when
there are no interionic interactions)
u+ (0+ ), u-(0- ) : mobility of cation & anion
z+, z- : charge of cation & anion

Infinitely dilute solutions - “Kohlrausch 2” law:  = + + -

 , + , - : Limiting equivalent conductivity of solution and ions
(-1.eq-1.cm2)
Note: ∞ (acids) > ∞ (bases) >> ∞ (salts)
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 MOBILITY OF H + & OH -

– oH+ and oOH- are very high comparing with

orthers o .10 5
Ion (cm2.s-1.V-1)
– Reason: (@ 25oC)

In electric field, H+ and OH- transport in aqua H+ 363

solutions following the “chain” mechanism
OH- 205
H+ + H2O  H3O+
H H
Na+ 52
H H
H-O-H + O-H  H-O + H-O-H
+ +
Cl- 79
H H H H
H-O + O-  O- + H-O
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Electrical conductivity vs. solvent

Relative Max
Solvent (HCl)
permittivity (25 oC)
(D)
H2O 81 394
CH3OH 31.2 117
C2H5OH 25.8 27.2
C3H7OH 22.2 9.7
C4H9OH 28.2 4.0
(C2H5)2O 4.4 0.04
 Method for measurement
of electrical conductivity
- Using “Wheatstone bridge”:
When G=0: R1/R2= R3/Rx

- (In lab) using conductivity meter:

 Applications
- Determine energy requirement for electrolysis process

- Determine salt’s concentration in solutions

- Determine solubility of relatively insoluble substances

- In analytical chemistry: Electrical conductivity analysis

 Electrical conductivity analysis

HCl by Weak acid Mixtures KCl by

NaOH by NaOH of strong/ AgNO3
weak
acids by
NaOH
Principle:
Due to the especially high conductivity of H+ and
OH- the equivalent volume can be recognized.
 5. ION TRANSPORT NUMBER

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 TRANSPORT NUMBER

• The transport number, t±, is defined as the fraction of total current

carried by the ions of a specified type.
qi
ti  Electrolyte KCl NaCl LiCl HCl
 qi t+ + t- = 1
tCl- (25oC) 0.506 0.604 0.670 0.170
q I  v 
t    
q  q I    
q I v 
t      
q  q I    

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 TRANSPORT NUMBER
The limiting transport number, t °, is defined in the same way


but for the limit of zero concentration of the electrolyte solution

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 HITTORF’S METHOD FOR
DETERMINATION OF TRANSPORT NUMBER
Principle: Determine ti via the concentration change in anode and cathode zones

Sơ đồ: Electrolysis of HCl, Pt inner electrodes

Anodic zone Middle zone Cathodic zone

Before
electrolysis

During
electrolysis

After
electrolysis

70