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Model Drude applied in ionic solutions

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Model Drude applied in ionic solutions

Vanessa Werlang1 , Nicole D. C. Lebrao1 , Erica R. L. R. Watanabe1 , Mauricio A. Ribeiro1 ,
Jessica R. P. Oliveira1 , Ervin K. Lenzi3 , Andressa Novastki3 ,
Lariana N. B. Almeida2 , Giane G. Lenzi1?

1 Universidade Tecnologica Federal do Parana - Parana (UTFPR), Ponta Grossa/PR,84016-210/

Brazil
2 Universidade Estadual de Maringa- Maringa/PR, 87020-900/ Brazil
3 Universidade Estadual de Ponta Grossa- Ponta Grossa/PR, 84030-900/Brazil.

? Corresponding Author: gianegoncalves@hotmail.com

Abstract. In this study presents a theoretical and experimental approach to the diffusion of ions and
conductometry of ionic solutions. The bases used the related theory of mass transfer, diffusion, of
ionic solutions and ionic conductometry. Potassium acetate and tribasic sodium citrate salts at differ-
ent temperatures (20◦C, 25◦C, 35◦C) were used to study the mobility of ions. The results indicated a
different electrical response that means a distinct behavior of ions when in aqueous solutions of pure
salts or mixtures. The study verifies that the mixture of solutions and the temperature directly influ-
enced the conductivity. For the temperature of 20◦C the result of the sequence for the conductivity as
a function of time was: 10% ethyl acetate - 90% citrate > 90% ethyl acetate - 10% citrate > 50% cit-
rate - 50% acetate > citrate > acetate; to a temperature of 25◦C to approximately sequence is: citrate
> acetate > 50% ethyl acetate - 50% citrate > 90% ethyl acetate - 10% citrate > 10% ethyl acetate -
90% citrate (up to 10 min) and 35◦C conductivity versus time was the following: 10% ethyl acetate
90% citrate > 50% citrate 50% acetate > citrate > 90% acetate - 10% citrate > acetate. Moreover,
the experimental data obtained were adjusted to the model proposed by Drude.

1 Introduction

The dynamics of inorganic salt ions in aqueous solution depends on several factors, such as ther-
modynamic, molecular, and structural, among others. In this sense, the diffusion phenomena and of
transport possible to gain magnitudes that macroscopic point of view allow the understanding of var-
ious aspects linked to moving ionic. Room temperature ionic liquids (RTILs) have been promoted as
the green and designer solvents of the next generation [1]. Physical properties of RTILs must be avail-
able for process design and development in their applications. However, there are very few data of
2019 Mathematics Subject Classification: 76R50, 60R60, 74F20, 74E30, 47N60, 80A50
Keywords: Diffusion, Ionic Solutions, Mixture of solutions.
2 Werlang et. al.

diffusion coefficients of ionic liquids in solvents, even in water [2, 3]. The mobility of ions is observed
in different areas, for example in the chemical industry [4, 5] and pharmaceutical products (treatment
of conservation of food) [6, 5, 7]. Application of this type of system can be useful in engineering to
check the purity of water to determine the content of substances gemstone dissolved in water (salin-
ity of the sea) and provide the determination of the concentration of electrolytes simple solutions.
Furthermore, this type of study has shown relevance in evaluating the dissolution of particles of salts
in drilling fluids pre-salt oil, with the modeling and determination of the coefficient of mass transfer
of salt particles in the disposal of the brine. Being this one way of minimizing the problems during
drilling, as the accumulation of the rubble of salt in the bottom of the pit, the weakening and enlarge-
ment of the pit walls and until the collapse of these walls [8, 9, 10]. Paul Drude performed called
intensive studies on the optical properties of a large number of materials. By combining these data
with the theory of electrons which was quickly established after J.J. Thomson’s experiment in 1897,
Drude standard explains the electrical conductivity, the thermal conductivity, and the optical proper-
ties of metals. The model he proposed in a series of papers published in 1900 off by typing metals
the classical gas of electrons executing the diffusive motion [11, 12, 13, 14]. Accordingly electronic
interaction is neglected, and scattering it repeats only on obstacles like ions, impurities etc.
In this way, the present work had as objective to assist the understanding of the dynamics of ions
(potassium acetate and sodium citrate) in aqueous solution. Being composed of a salt dissolved or
mixture of a salt dissolved, seeking a relationship between the macroscopic greatness that is mea-
surable (conductivity) models and the relevant microscopic description of these ions. In addition, the
behavior of the model of Drude will be evaluated for liquid systems.

2 Experimental Procedure
The experiment was carried out in an apparatus as shown in Fig. 2

Fig. 1: Experimental apparatus, (A) Diffusion Cell; (B) Becher jacketed; (C) Conductivity; (D). Cool-
ing / heating;(E) stirrer.

Is the diffusion study behavior of two different salts in aqueous solutions and admixtures of two
salts. The system works with the diffusion cell with 317 little capillary tubes, the diffusion cell is dis-
 Drude Model 3

posed on 1L-becker with 700 mL of ultrapure water, the becker is on a magnetic stirrer to homogenize
the liquid to be registered with a conductivity. The aqueous solutions were disposed at the diffusion
cell to can be studied. The salts used were: Potassium acetate (C2 H3 KO2 ) (by Perquin79.5% purity)
and sodium citrate (tribasic) (Na3C6 H5 O7 .2H2 O) (by Perquin> 79.5%purity) in aqueous solution 0.1
M. The salts were chosen due to structural difference of molecule. The potassium acetate is salt,
which has high solubility in water 253 g/100ml at 20◦C, is an alkaline solution pH of 9.7. Figure 2A
indicates the molecular structure of potassium acetate. The sodium citrate is an organic product in the
form of crystals, it is water soluble and insoluble in ethyl alcohol, its structure can be found in Figure
2B.

Fig. 2: The molecular structure A) potassium acetate (B) sodium citrate (tribasic).

The mixture of the salts was prepared in the following proportions of sodium citrate (tribasic)
50%- potassium acetate 50%(50 − 50%Ac : Cit); 90% tribasic sodium citrate -10% Potassium acetate
solutions (90 − 10%Ac : Cit)and 10% tribasic sodium citrate - 90% of potassium acetate (10 − 90%
Ac:Cit), 0.1 M. The tests were performed opened to the air is 35 minutes.

2.1 Model of Drude

The model of Drude was applied to adjust the results of conductivity versus time in aqueous solution
[13, 15, 16, 17]. We base our review of the results of the equations:
d
mi vi = −αi vi + qI E (2.1)
dt
Rewrite the Eq. 2.1, thus:

d αi qI
vi = − vi + E (2.2)
dt mi mi
dvi
where I refer to the type of this ion in aqueous solution. Considering, dt = 0, defines the stationary
solution of the equation 2.1, thus:
4 Werlang et. al.
qI
v̂i = E (2.3)
αi
The solution of the above equation is
 αt
− i
vi = qi E/mi )(1 − e mi )(2.4)

and the same must be used to compose the current density given by the following equation below.

J = ∑ Ni qi vi (2.5)
i

Substituting Eq. 2.4 into Eq. 2.5, we have:

Ni q2i E αt
− i
J=∑ (1 − e mi ) (2.6)
i mi
Rewrite Eq. 2.6, thus:

N1 q21 E α t
− 1 N2 q22 E α t
− 2
J= (1 − e m1 ) + (1 − e m2 ) (2.7)
m1 m2
Using the equation above and the fact that current density and the field can be related through the
equation [18, 19, 20]. We get the conductivity is given by

Ni q2i
σ(t) = ∑ (1 − e−αit/mi ) (2.8)
mi
Thus, rewrite the Eq. 2.8

N1 q21 N2 q22
σ(t) = (1 − e−α1t/m1 ) + (1 − e−α2t/m2 ) (2.9)
m1 m2
For fit of the experimental data with equation and adjustment, the least squares method is used to
analyze its behavior. Likewise, the quality of the adjustment was analyzed by the Person Coefficient
R2 , defined by the following equation:

cov(X,Y )
R= p (2.10)
var(X)var(Y )

where cov(X,Y ) is the covariance between experimental data and model give Eq. 2.9, var(X) is the
variance of experimental data and var(Y ) is the variance of model data. For the analyzed cases the
behavior of the Pearson coefficient was satisfactory, i. e., values close to 0.998.

3 Experimental Results

Figs.3 Present the results of conductivity in function of time for different temperatures, for the potas-
sium acetate and pure sodium citrate in aqueous solution. Figs. 4, 5 and 6 show the behavior of
conductivity in function of time for the temperature of 20, 25 and 35◦C for pure salts and mixtures.
The table 1, 2 and 3 present the values of the parameters of the model Drude for the temperatures 20,
25 e 35◦C, respectively.
 Drude Model 5

3.1 Behavior of pure salts with temperature increase

To better evaluate the behavior of conductivity in the mixture of salts the experiments were performed
with the salts pure, the results are presented in Fig. 3, for the (A) potassium acetate and (B) Sodium
citrate, respectively.

1 0 3 5

9
A 3 5 C
o B
3 0 o
3 5 C
8

7 2 5

o
C o n d u c t i v i t y ( µS )

C o n d u c t i v i t y ( µS )
6 2 5 C
2 0
5
o
1 5 2 5 C
4 o
2 0 C
3 1 0

2
o
5 2 0 C
1

0 0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0 0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
T im e ( m in ) T im e ( m in )

(a) Potassium acetate (b) Sodium citrate

Fig. 3: Graph of conductivity (A) Potassium acetate (B) Sodium citrate, at different temperatures.

The results indicated, as expected, that with the increase of temperature occurred an increase of
conductivity, for the two studied salts. However, for the potassium acetate (Fig. 3A) occurred a behav-
ior of instability of the experimental data. Being the largest conductivity obtained was 9.27µS(35◦C).
In Figure 3B, it was observed a greater difference in value of conductivity between the readings 20
and 25 ◦CC and by the format of the chart is clear how much the actuation of Temperature modi-
fies the dissemination, because the graph at a temperature of 20◦C Demonstrates that the process of
diffusion slow in comparison with the other temperatures studied. This is due to the ions have less
energy to carry out the movement of diffusion. We realized that the acetate solution when compared
with the citrate solution, suffers less influence of temperature, because the averages, acetate solution,
the increase of 20 to 25◦C were approximately 35% and of 25 to 35◦C approximately 57%. So it can
realize the greatest response of acetate was in the increase of the only 5◦C when the temperature is
increased 10◦C it was expected a more significant increase. The citrate already had a significantly
higher response to temperature changes when compared to pure acetate, because to compare the read-
ings of the conductivity of pure acetate solution, note that the values obtained the temperature 35◦C
only doubled when compared with the values verified the 20◦C. In the case of the citrate, they were
very high reaching almost 6 times increase when compared to the measurements of 20◦C and of 35◦C.
This may have happened due to the much larger number of ions present in the citrate solution because
to provide more energy there was an increase in the movement ionic.

4 Analysis of the mixture of salts in the same temperature

The obtained results of conductivity versus time to the mixture of salts to the temperature of
20◦C(concentration of 0.1M ) is shown in Fig.4. Continuous lines indicate the adjustments made
by using the model of Drude.
6 Werlang et. al.

1 4
1 3 (a )
(b )
1 2
(c )
1 1 (d )
1 0 (e )
9
C o n d u tiv ity ( µ S )

8
7
6
5
4
3
2
1
0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
T im e ( m in )

Fig. 4: Behavior of conductivity in function of time, T=20◦C, (a) acetate; (b) citrate; (c) mixture 50%
acetato-50%citrato (d) mixture 10% acetate-90% citrate (e) mixture 90% acetate-10% citrate

As can be observed in Figure 4 (d), the mixture 10% acetate -90% citrate was that obtained the
highest conductivity. This indicates the greater interaction between the free and the water ions, which
led to an increase in the mobility of ions (conductivity). Is mobility was more pronounced with a
greater amount of sodium citrate (that pure, in relation to the acetate, presented a greater conductivity).
Another observation was that the values of conductivity increased in time studied more between
mixtures of that pure substances. Soon, we can conclude that the ions interact among themselves by
modifying the disabled. The mixture 50% − 50%, in 35 minutes has obtained an intermediary value
between the citrate and pure acetate. The conductivity in function of time has followed the sequence:
10%acetate-90%citrate > 90% acetate-10% citrate> 50% acetate-50%citrate>citrate>acetate. The
parameters found for mixtures and pure solution, are shown in Table 1.

Table 1: Parameters of the adjustments by the model of Drude. (T = 20◦C)

N1 q21 α1 N1 q21 α1
Electrolytic Solutions m1 m1 m1 m1
Pure acetate 1.62347 -0.0874939 3.09827 -0.0874939
Pure Citrate 5.56802 -0.0281135 5.6709 -0.0281135
50% acetate-50%citrate 3.18335 -0.176089 50.6557 -0.00129062
10% acetate-90% citrate 2.55373 -3.37899 11.9491 -0.0690025
90% acetate-10% citrate 0.542517 -1.07348 6.6496 -0.0761714

For the coolant temperature to 25◦C (Fig.5), It is noticed a different behavior of previously sub-
mitted (Figure 4). With an increase in the temperature of the system, there was a sharp increase in
 Drude Model 7

2 0

1 8

1 6

1 4 (a )
(b )
C o n d u tiv id a d e ( µ S )

1 2 (c )
(d )
1 0
(e )
8

0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
te m p o ( m in )

Fig. 5: Behavior of conductivity in function of time, T=25◦C, (a) acetate; (b) citrate; (c) mixture 50%
acetato-50%citrato (d) mixture 10% acetate-90% citrate (e) mixture 90% acetate-10% citrate

conductivity in the studied period for the solution of sodium citrate. The values described in the liter-
ature for the mobility of the ion K+ and Na+ are i=73.50 ohm/eq and i=50.10 ohm/eq, respectively.
Thus, it is expected that the substance that contains potassium ions have a higher conductivity that
the substance of sodium, however, we must take into account the influence of the molecular struc-
ture of sodium citrate and potassium acetate. This suggests that the long molecule of sodium citrate
(Na3 (C3 H5 O(COO)3 ).2H2 O) may have a greater difficulty to spread, compared with the molecule of
potassium acetate (CH3COOK). Another difference of results obtained 20◦C Is that the solutions of
the mixture also presented conductivity less than the solution of potassium acetate, only with the ex-
ception the mixture 10% acetate-90% citrate Figure 5 (d) obtained some higher values than the acetate
solution. The conductivity in function of time followed the approximate sequence: citrate¿acetate
> 50% acetate-50% citrate > 90% acetate-10% citrate> 10% acetate-90% citrate (until ≈ 20 min).
After this period this sequence if modifies for the citrate > 90% acetate-10% acetate> 50% acetate-
50% citrate>citrate> 10% acetate-90% citrate. The parameters found for mixtures and pure solution,
are shown in Table 2

Table 2: Parameters of adjustments by the model of Drude. (T= 20◦C)

N1 q21 α1 N1 q21 α1
Electrolytic Solutions m1 m1 m1 m1
Pure acetate 3.0542 -1.23178 3.96762 -0.0250798
Pure Citrate 5.68797 -0.027699 5.66347 -0.0276991
50% acetate-50%citrate 1.36414 -0.763459 5.33014 -0.0377466
10% acetate-90% citrate 3.55144 -0.0457704 3.95623 -0.0457704
90% acetate-10% citrate 1.15403 -0.679524 3.13761 -0.0605834
8 Werlang et. al.

As expected, an increase in conductivity was observed with the increase of temperature (35◦C,
Fig.6). Note that the mixture 10% potassium acetate-90% Sodium citrate obtained the highest con-
ductivity in function of time, as well as in the temperature of 20◦C. On the other hand, it was observed
that the mixture 90% acetate-10% citrate and potassium citrate, were practically the same, indicating
that the small quantity of citrate added, not influence on conductivity, possibly due to the larger size
of the molecule. The conductivity in function of time has followed the sequence: 10% acetate-90%
citrate > 50% acetate-50% citrate > citrate > 90% acetate-10% citrate > acetate.

1 4
1 3 (a )
(b )
1 2
(c )
1 1 (d )
1 0 (e )
9
C o n d u tiv ity ( µ S )

8
7
6
5
4
3
2
1
0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
T im e ( m in )

Fig. 6: Behavior of conductivity in function of time, T=35◦C, (a) Potassium acetate; (b) citrate; (c)
mixture 50% acetate-50% citrate (d) mixture 10% acetate-90% citrate (and) mixture 90% acetate-10%
citrate.

In all the experiments the behavior of pure citrate in relation to the pure acetate was the same, i.e.
the citrate had higher conductivity this is the form of dissociation of a molecule of salt sodium citrate
which frees three ions of sodium and a citrate solution. Thus, have four ions to conduct an electrical
current in the solution, thereby increasing the conductivity. Already the decoupling of a molecule
potassium acetate only generates an ion acetate and a potassium ion.
As expected, an increase in conductivity was observed with the increase of temperature (35◦C,
Fig.6). Note that the mixture 10% potassium acetate-90% Sodium citrate obtained the highest con-
ductivity in function of time, as well as in the temperature of 20◦C. On the other hand, it was observed
that the mixture 90% acetate-10% citrate and potassium citrate, were practically the same, indicating
that the small quantity of citrate added, not influence on conductivity, possibly due to the larger size
of the molecule. The conductivity in function of time has followed the sequence: 10% acetate-90%
citrate > 50% acetate-50% citrate > citrate > 90% acetate-10% citrate > acetate.
In all the experiments the behavior of pure citrate in relation to the pure acetate was the same, i.e.
the citrate had higher conductivity this is the form of dissociation of a molecule of salt sodium citrate
 Drude Model 9

Table 3: Parameters of adjustments by the model of Drude. (T= 35◦C)

N1 q21 α1 N2 q22 α2
Electrolytic Solutions m1 m1 m2 m2
Pure acetate 9.12048 -0.115185 - -
Pure Citrate 22.0516 -0.437878 13.5389 -0.0375147
50% acetate-50% citrate 67.0418 -0.230718 - -
10% acetate-90% citrate 73.8604 -0.73955 - -
90% acetate-10% citrate 4.23691 -2.62266 4.33121 -0.113377

which frees three ions of sodium and a citrate solution. Thus, have four ions to conduct an electrical
current in the solution, thereby increasing the conductivity. Already the decoupling of a molecule
potassium acetate only generates an ion acetate and a potassium ion.

Table 4: Parameters of adjustments by the model of Drude. (T= 35◦C)

N1 q21 α1 N2 q22 α2
Electrolytic Solutions m1 m1 m2 m2
Pure acetate 9.12048 -0.115185 - -
Pure Citrate 22.0516 -0.437878 13.5389 -0.0375147
50% acetate-50% citrate 67.0418 -0.230718 - -
10% acetate-90% citrate 73.8604 -0.73955 - -
90% acetate-10% citrate 4.23691 -2.62266 4.33121 -0.113377

The analysis of the mixture 50% acetate -50% citrate to 20◦C and 35◦C, presented behaviors in-
teresting. A first expectation was to have an average behavior, i.e., the conductivity of the mixture to
be between the conductivity of pure salts, tabled by both pure solutions and mixtures, 20◦C It is per-
ceived that their behavior was matched when compared with the solutions of citrate and pure acetate.
However at 35◦C its conductivity was much greater than expected, staying next when the mixture
10% acetate-90% citrate, That was the one that showed higher conductivity at temperatures of 20
and 35◦C. This probably occurred due to the facilitation of the ionic movement due to the presence
of different ions facilitated this migration of ions, besides the increase of temperature. Already in the
case of mixtures 10% acetate-90% citrate Both the temperature of 20 and 35◦C presented greater con-
ductivity both compared with the pure substances and mixtures, which demonstrates that the presence
of more ions, probably increases the speed of diffusion due to the ionic movement. In the study of
mixtures 90% acetate-10% citrate, It is noticed a distinct behavior, because the behavior presented the
20◦C, Is higher than expected, since their composition has more ions of potassium acetate, foresaw a
behavior more similar to that of the pure acetate as occurred in the experiment conducted the 35◦C.
This may have occurred due the presence of sodium citrate ions in small quantity helped the ionic
movement at 20◦C. Already the 35◦C, due to the small quantity of sodium citrate ions and there was
no significant difference in the diffusion of the mixture when compared with the pure acetate solution.
10 Werlang et. al.

4.1 Analysis of the influence of the temperature of the Mixture

50% Potassium acetate -50% Sodium citrate

The results obtained for the conductivity of the mixture 50% acetate -50% performed the citrate 20◦C
with error of ± 1.91◦C,the 25◦C with an error of ± 0.27◦C and the 35◦C was performed with error ±
0.31 ◦C. The behavior of the solution can be found in Figure 7A. The measures of the mixture 10%
acetate-90% citrate Were performed at 20◦C with an error of ± 1.27◦C, the of 25◦C with an error of
± 0.2◦C and the reading of 35◦C was performed with error ± 0.03 ◦C, Figure 7B . The obtained data
20◦C with an error of ± 1.14◦C, the of 25◦C with an error of ± 0.0◦C and the obtained data 35◦C
with an error of ± 0.27 ◦C, Figure 7C.

1 0 0
1 4
(a ) (a ) (d )
1 3 9 0 (b ) (e )
(b ) (c )
1 2
(c ) 8 0
1 1 (d )
1 0 (e ) 7 0

9
C o n d u tiv ity ( µ S )

6 0

C o n d u tic ity ( µ S )
8
7 5 0

6 4 0
5
3 0
4
3 2 0
2
1 0
1
0 0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0 0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
T im e ( m in ) T im e ( m in )

(a) Potassium acetate (b) Sodium citrate

o
T = 3 5 C
7 0 A
6
6 0
5
o
T = 2 0 C
5 0 4
o
T = 2 5 C
C o n d u tiv ity ( µ S )

4 0
2

3 0
0
0 2 0 4 0

2 0

1 0 o
T = 2 0 C
o
T = 2 5 C

0
0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 0
T im e ( m in )

(c) Sodium citrate

Fig. 7: Graph of conductivity A) 50% citrate and 50%B) 10%acetate-90% citrate C) 90% acetate-10%
citrate.

For the mixture 50% acetate- 50% citrate, checks on the graph values obtained in reading the 35◦C
are much higher when compared to that of other temperatures studied, and the values obtained for 20
and 25◦C, many were closer. You can see in detail the graph Figure 4A, that. On the other hand,
the values obtained for the conductivity in temperature of 25◦C are smaller than the temperature of
20◦C. For the mixture 10% acetate-90% citrate, you can see a big difference in the behavior of the
temperature of the ions 35◦C because the values of conductivity are much higher than those obtained
25◦C and 20◦C (Figure 4B). This is due to the increase of energy of ions, with greater mobility for
 Drude Model 11

the diffusive flux movement. Furthermore notes that conductivity at the temperature of 20◦C obtained
higher values than the conductivity of reading the 25◦C. We can see a clear influence on conductivity
in the mixture 90% acetao-10% citrate, In relation to the concentration, where it was obtained a
difference between the data, and the temperature of 20◦C Obtained values higher than 25◦C.

5 Conclusions

The mixture of solutions directly influences the conductivity, as is indicated in the sequences for
the temperature of 20◦C: 10% acetate -90% citrate >90% acetate-10% citrate¿50% acetate-50%
citrate>citrate>acetate; for the temperature of 25◦C The conductivity in function of time followed the
approximate sequence: citrate>acetate >50% acetate-50% citrate >90% acetate-10% citrate>10%
acetate-90% citrate (until ≈ 10 min) And for the temperature of 35◦C The conductivity in function of
time has followed the sequence: 10% acetate-90% citrate >50% acetate-50% citrate > citrate >90%
acetate-10% citrate > acetate . The direct influence of the concentration in the mobility of potassium
citrate ions and sodium acetate, under the conditions and mixtures, studied, where temperature 20◦C
has the conductivity higher than for 25◦C. The model of Drude is applicable, in addition to solid
systems (metals) already indicated in the literature, in liquid systems (electrolytic solutions).

Acknowledgements

The authors acknowledge support by CNPq, CAPES and FA, all Brazilian research funding agencies.
The M.A. Ribeiro thanks CNPq for finantial support.

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