Volume 02 Issue 10-2022
25
American Journal Of Applied Science And Technology
(ISSN
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2771-2745)
VOLUME
02
I
SSUE
10
Pages:
25-34
SJIF
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(2021:
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1121105677
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Servi
ABSTRACT
The article studies the influence of parameters on the reaction rate of catalytic dimerization of methane, kinetic
relations in the flow differential quartz reactor (P=0,1 MPa, Vcat =0.5÷2 ml, СН4:О2=2:4, contact time 0.1÷0.09 sec) i
n
the temperature range of 750-580
℃
. The influence of temperature on methane conversion and product selectivity,
the influence of oxygen and hydrogen impurities on methane conversion and acetylene selectivity, and the
dependence of ethane selectivity on temperature were discussed. At different concentrations of methane with a
volume
ratio of СН4:О2=3:1 in the mixture, the influence of temperature parameters on selectivity for acetylene was
studied, a reaction mechanism was proposed and a kinetic model was developed for obtaining ethane, ethylene,
acetylene and acetic anhydride from methane.
KEYWORDS
Methane, ethane, ethylene, acetylene, catalyst, kinetic equation, mechanism, contact time, dimerization.
Research Article
THE KINETICS OF THE METHANE DIMERIZATION REACTION
Submission Date:
October 01, 2022,
Accepted Date:
October 05, 2022,
Published Date:
October 14, 2022
Crossref doi:
https://doi.org/10.37547/ajast/Volume02Issue10-05
Safarova Mavjuda Jomurodovna
Samarkand State University, 15 University Boulevard, Samarkand, 140104, Uzbekistan
Normurot Ibodullayevich Fayzullaev
Samarkand State University, 15 University Boulevard, Samarkand, 140104, Uzbekistan
Journal
Website:
https://theusajournals.
com/index.php/ajast
Copyright:
Original
content from this work
may be used under the
terms of the creative
commons
attributes
4.0 licence.
Volume 02 Issue 10-2022
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American Journal Of Applied Science And Technology
(ISSN
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2771-2745)
VOLUME
02
I
SSUE
10
Pages:
25-34
SJIF
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(2021:
5.
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(2022:
5.
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OCLC
–
1121105677
METADATA
IF
–
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Publisher:
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Servi
INTRODUCTION
Currently, the demand for petrochemical
products is increasing worldwide. Vinyl chloride,
polyethene, ethylene oxide, vinyl acetate, lavsan,
etc. are in high demand. The main raw material
for all the above-mentioned substances is
ethylene. Currently, ethylene is mainly produced
by the thermal decomposition of gasoline. The
dynamic growth of demand for motor fuels is
pushing to find another innovative way to obtain
the main organic synthesis product. One such
innovative method is the catalytic dimerization of
methane to ethylene [1-6].
At the same time, ethylene extraction from
methane has not been established. The main
reason for this is that the equipment for the
process is not equipped and the optimal mode is
not selected. It is necessary to study the kinetic
laws of the reaction transition to determine the
appropriate mode and equip the devices.
Several works have been published [7-11] on the
catalytic oxidative transformation of methane,
and various absorbed catalysts have been
proposed for the production of ethylene and
ethane from methane. The peculiarity of the
methane oxidation condensation reaction is that
in all known catalysts the reaction takes place at
a high temperature and the process is strongly
exothermic. In addition, the CH
4
+ O
2
mixture has
strong explosive properties. At the same time, the
activity and selectivity of catalysts are low.
In addition, the kinetics of the methane
dimerization reaction in the catalysts of all
studied literature Bi
2
O
3
∙9% K
2
CO
3
/Al
2
O
3
; 34%
PbO/Al
2
O
3
; 4% Na
2
MoO
4
*10%Mn-O/SiO
2
has not
been fully studied without taking into account the
processes involving catalysts. In the reactions
with the mentioned catalysts, formal rank
equations were used for the kinetic expression of
the process. In all works, ethylene was obtained
as the target product [12-19].
Prospects for the practical application of the
catalytic dimerization of methane.
The yield of
С
2
hydrocarbons strongly depends on the content
of CH
4
+ oxygen in the reaction mixture. To obtain
С
2
-hydrocarbons in high yield, it is necessary to
use a non-diluted reaction mixture. It is better to
have a volume ratio of CH
4
/O
2
=4-5.
The practical implementation of the catalytic
dimerization reaction of methane has the
following difficulties:
1) As a result of the reaction, ethane, ethylene,
and a small amount of propane and propylene,
which are more reactive than methane, are
formed. The resulting products are completely
oxidized to CO
2
in the presence of a catalyst.
2) The reaction products react more easily with
oxygen than with methane in the gas phase.
Therefore, it is necessary to portion out oxygen or
quickly remove the reaction products from the
reaction zone.
3) A large amount of heat is released during the
catalytic dimerization of methane, which requires
efficient use [21-27].
MATERIALS AND METHODS
The reactor is a quartz tube with a length of 650
mm and an internal diameter of 8 mm. The size of
the catalyst is 0.25-0.5 mm. To reduce the volume,
quartz crystals were placed on the bottom and on
top of the catalyst. The catalytic activity of the
catalyst in a flow differential quartz reactor
Volume 02 Issue 10-2022
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American Journal Of Applied Science And Technology
(ISSN
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VOLUME
02
I
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10
Pages:
25-34
SJIF
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FACTOR
(2021:
5.
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(2022:
5.
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OCLC
–
1121105677
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(P=0.1 MPa, Vkat=0.5 ml÷2 ml, CH
4
:O
2
=2÷4,
contact time 0.1-0.09 sec) in the temperature
range of 750-
850 ℃ studied [23, 21
-26].
The temperature was changed in the range from
700 to 850 ℃. Under the given conditions,
the
conversion of methane varies from 1 to 35%, and
the conversion of oxygen varies from 4 to 98%.
The selectivity for reaction products varies from
30 to 70%.
99.9% pure methane and pure oxygen were used
for the reaction. The gases were mixed before
entering the reactor. A laboratory device with a
flow differential reactor was created to study the
kinetic laws of the methane oxycondensation
reaction.
The gas products of the reaction were
chromatographically
analyzed
using
a
thermochemical detector with an additional
thermostat "Gazochrom3101" was analyzed in a
chromatograph under the following optimal
conditions: column thermostat temperature -100
℃, carrier gas (air) flow rate
-35 ml/min, column
length filled with activated carbon - 1 m, internal
diameter - 3 mm. Quantitative analysis was
performed using the absolute ranking method
[20, 21-24].
Results and discussion
The effect of some parameters on the rate of
catalytic dimerization of methane was studied.
The obtained results are presented in Figure 1.
Figure 1. Effect of temperature on methane conversion and product selectivity
Figure 1 shows the temperature dependence of
the conversion of methane (X) and the selectivity
of the formation of reaction products. As can be
seen from Figure 2, the conversion of methane
starts at 600
℃. The first product of the oxidative
dimerization reaction of methane is ethane and a
small amount of ethylene. When the temperature
is further increased, the selectivity of the
formation of ethane and ethylene increases, and
the selectivity to ethane reaches a maximum of
800 ℃. At 800 ℃, the selectivity of ethane is about
2 times higher than the selectivity of ethylene. But
820-830
℃
the selectivity of all products drops
sharply. After the temperature exceeds 8000,
peaks (rounds) characteristic of acetylene
appears in the chromatograms. Temperature
850
℃
after exceeding, its selectivity increases
sharply. Also, the selectivity of the formation of
Volume 02 Issue 10-2022
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VOLUME
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I
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5.
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ethane and ethylene is 900
℃
reaching the second
maximum at
Figure 2 below examines the effects of oxygen and
hydrogen additions on methane conversion and
acetylene selectivity.
Figure 2. Effect of oxygen and hydrogen additions on methane conversion and acetylene
selectivity
In oxidative dimerization, the conversion of
methane in the desired composition of the
reaction mixture is 600
℃
starts from and
increases with increasing temperature. When the
concentration of oxygen in the initial reaction
mixture is increased, the conversion of methane
increases.
Figure 3. Dependence of selectivity on ethane on temperature.
The conversion of methane is almost unchanged
when hydrogen is added to the initial reaction
mixture. At this time, the formation of the first
product of the reaction, ethane, does not depend
on the reaction conditions. Ethane 680-700 when
we carry out the reaction in the absence of oxygen
(line 3). And in the presence of oxygen (CH
4
:O
2
=
3:1 and CH
4
:O
2
= 2:1; lines 4 and 5) 650
℃
is
formed in When obtained in CH
4
:H
2
= 1:1 and
Volume 02 Issue 10-2022
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American Journal Of Applied Science And Technology
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VOLUME
02
I
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Pages:
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5.
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CH
4
:H
2
= 1:2 ratios (lanes 2 and 1) 700
℃
begins
to form. Under these conditions, the selectivity to
ethane is 750
℃
will be the maximum.
Figure 4. Effect of temperature on acetylene selectivity for different concentrations of methane in
CH
4
:O
2
=3:1 mixture
As can be seen from the figure, when the effect of
temperature on the selectivity for acetylene is
studied for methane concentrations of 15%, 30,
45, and 60% in the CH
4
:O
2
=3:1 mixture, the
selectivity to acetylene increases as the
concentration of methane in the mixture
decreases.
Based on the results obtained
we will consider the mechanisms and kinetic
models of chain reactions.
A reliable mechanism for the formation of ethane
from methane can be expressed as follows:
Volume 02 Issue 10-2022
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VOLUME
02
I
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Pages:
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1121105677
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2Z + O
2
𝑘
1
→
2ZO; 2ZO + CH
4
𝑘
2
→
ZOCH
3
+ ZOH; ZOCH
3
+ CH
4
𝑘
3
→
C
2
H
6
+ ZOH
2ZOH
𝑘
4
→
H
2
O + ZO + Z
0,5O
2
+ 2CH
4
→
C
2
H
6
+ H
2
O
Under the condition of stationarity, W1 = W2 =
W3 = W4 and the total number of surface areas is
constant (∑i =1), the equation for the rate of
ethane formation according to the above
mechanism is as follows:
𝜃
𝑊
𝐶
2
𝐻
6
=
𝑘
3
2
𝑃
𝐶𝐻
4
4𝑘
2
{
−
(
√
𝑘
2
𝑃
𝐶𝐻
4
𝑘
1
𝑃
𝑂
2
+ √
𝑘
2
𝑃
𝐶𝐻
4
𝑘
4
+ 1
)
+ √(√
𝑘
2
𝑃
𝐶𝐻
4
𝑘
1
𝑃
𝑂
2
+ √
𝑘
2
𝑃
𝐶𝐻
4
𝑘
4
+ 1)
2
+ 4
𝑘
2
𝑘
3
}
The chain mechanism of the formation of ethylene from ethane:
C
2
H
6
𝑘
5
→
2
𝐶𝐻
3
∎
;
𝐶𝐻
3
∎
+ C
2
H
6
𝑘
6
→
CH
4
+ C
2
𝐻
5
∎
; C
2
𝐻
5
∎
𝑘
7
→
C
2
H
4
+ H
2
𝐻
∎
+
C
2
H
6
𝑘
8
→
𝐶
2
𝐻
5
∎
+ H
2
; 2 C
2
𝐻
5
∎
𝑘
9
→
C
2
H
4
+ C
2
H
6
; 2 C
2
𝐻
5
∎
𝑘
10
→
C
4
H
10
2𝐶𝐻
3
∎
𝑘
11
→
C
2
H
6
; C
2
H
6
→ C
2
H
4
+H
2
The equation for the reaction of ethylene formation according to the above mechanism:
𝑊
𝐶
2
𝐻
4
= 3𝑘
6
𝑃
𝐶
2
𝐻
6
(1 −
0.33
1+
𝐾8
𝑘9
)
+
𝑘
5
(
𝑘7
𝑘9
)
1/2
(1+
𝑘8
𝑘9
)
1/2
𝑃
𝐶
2
𝐻
6
1/2
It was also found that the contact gases contained CO
2
. CO
2
is mainly formed by the interaction of a
weakly adsorbed oxygen molecule with methane:
O
2
+ Z
𝑘
1
∗
→
O
2
Z; CH
4
+ Z
𝑘
2
∗
→
CH
4
Z; ZCH
4
+ 2ZO
2
𝑘
12
→
2CO
2
+ 2H
2
O + 3Z
The reaction rate of CO
2
formation:
𝑊
𝐶𝑂
2
=
2𝑘
12
𝐾
1
∗
𝑃
𝑂
2
𝐾
2
∗
∙ 𝑃
𝐶𝐻
4
(1 + 𝐾
1
∗
∙ 𝑃
𝑂
2
+ 𝐾
2
∗
∙ 𝑃
𝐶𝐻
4
)
2
Carbon dioxide is formed from the interaction between a methane molecule and dissociatively adsorbed
oxygen:
2Z + O
2
𝐾
1
→
2ZO; 2ZO + CH
4
𝑘
13
→
CO + 2Z + H
2
+ H
2
O;
O
2
+ 2CH
4
→ 2CO + 3
H
2
+ H
2
O
The equation for the rate of formation of CO is:
𝑊
𝐶𝑂
= 𝑘
13
𝑃
𝐶𝐻
4
(
1
1 + √
𝑘
13
𝑃
𝐶𝐻
4
𝐾
1
𝑃
𝑂
2
)
2
The reaction rate constants were calculated according to the experimental results presented in Table 1.
Volume 02 Issue 10-2022
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VOLUME
02
I
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Pages:
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SJIF
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(2021:
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5.
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Table 1. Experimental test results
Temperature,
℃
Component concentration, % mol
H
2
CH
4
O
2
N
2
CO
2
C
2
H
4
C
2
H
6
CO
Contact time-2 s
700
1.9
24.8
0.8
56.8
2.4
8.7
1.3
0.4
730
0.8
25.6
1.1
57.3
3.6
8.0
1.2
0.3
735
1.8
24.6
1.8
57.4
2.8
8.0
1.2
0.3
750
4.6
26.2
1.7
53.3
3.4
8.5
0.7
1.3
750
3.8
22.4
1.5
58.6
3.9
8.0
0.8
1.1
800
8.4
24.0
0.3
49.8
3.5
8.0
0.2
3.8
850
14.8
23.7
0.2
42.0
2.2
6.9
0.0
8.1
Contact time-1 s
600
0.4
30.4
0.1
55.7
1.2
8.3
1.4
0.5
660
1.7
27.1
0.0
56.6
2.1
8.4
1.1
1.0
665
2.7
28.1
0.0
54.7
2.0
8.4
1.1
1.0
700
2.2
29.1
0.0
54.3
1.9
8.4
1.3
0.7
750
2.3
27.6
0.0
55.5
2.2
8.5
1.2
0.7
770
2.2
28.6
0.0
54.4
2.1
8.8
1.3
0.7
800
6.2
28.0
0.0
50.2
2.6
8.2
0.7
2.1
Contact time-0.5 s
615
2.8
26.1
1.0
56.1
1.3
5.8
0.8
2.0
650
3.9
27.2
0.0
54.1
1.7
6.0
0.6
2.6
700
3.2
27.6
0.0
54.6
1.4
5.9
0.6
2.3
750
2.8
27.2
0.0
55.6
1.5
6.0
0.6
2.3
800
5.1
28.9
0.0
51.3
1.9
5.9
0.6
2.4
800
3.7
24.9
0.0
56.1
1.5
5.8
0.5
3.3
850
4.3
24.6
0.0
55.7
1.6
5.8
0.4
2.5
In the catalytic dimerization of methane,
acetylene is formed from the oxidative
dehydrogenation of ethylene. At this time, the
dissociatively
adsorbed
oxygen
molecule
interacts with the ethylene molecule to form the
ZOC
2
H
4
complex. This in turn splits into acetylene
and water molecules:
2Z + O
2
𝑘
1
→
2ZO; ZO + C
2
H
4
𝑘
14
→
ZOC
2
H
4
; ZOC
2
H
4
𝑘
15
→
C
2
H
2
+ H
2
O + Z
0.5O
2
+ C
2
H
4
→ C
2
H
2
+ H
2
O
According to this mechanism, the rate of formation of acetylene:
Volume 02 Issue 10-2022
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VOLUME
02
I
SSUE
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Pages:
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SJIF
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(2022:
5.
705
)
OCLC
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𝑊
𝐶
2
𝐻
2
=𝑘
1
𝑃
𝑂2
[
−1 + √1 + 4 (
𝑘
1
𝑃
𝑂
2
𝑘
14
𝑃
𝐶
2
𝐻
4
+
𝐾
1
𝑃
𝑂
2
𝑘
15
)
2 (
𝑘
1
𝑃
𝑂
2
𝑘
14
𝑃
𝐶
2
𝐻
4
+
𝑘
1
𝑃
𝑂
2
𝑘
15
)
]
2
The above equations constitute the kinetic model of the process.
The parameters of the kinetic models were determined based on the experimental results using the
following objective function:
𝐹(𝑥) = ∑ [
𝐴
expe
− А
𝑎𝑐𝑐.
𝐴
expe
]
2
𝑁
1
where x is the kinetic parameter of the considered
model;
𝐴
expe
А
𝑎𝑐𝑐.
-experimental and calculated
values of the yield of reaction products; Number
of N-components.
The created kinetic model of the methane
oxidation condensation reaction adequately
represents the experimental values (the relative
error of the experimental and calculated values
does not exceed 10%).
CONCLUSION
Thus, the factors affecting the rate of the catalytic
oxidation dimerization reaction of methane, the
kinetic laws of the reaction in a flowing
differential quartz reactor (P = 0.1 MPa, V
cat
= 0.5
ml÷2 ml, CH
4
:O
2
= 2÷4, contact time 0, 1-0.09 sec)
was studied in the temperature range of 750-850
℃.
Effect of temperature on methane conversion
and selectivity of products, the effect of oxygen
and hydrogen additives on methane conversion
and selectivity on acetylene, and temperature
dependence of selectivity on ethane, Based on the
study of factors such as the effect of temperature
on the selectivity for acetylene in the mixture
CH
4
:O
2
=3:1, the mechanism of the reactions of the
formation of ethane, ethylene, acetylene, and
carbon dioxide from methane was proposed and
a kinetic model was created.
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1.
Daneshpayeh M., Khodadadi A., Mostoufi N.,
Mortazavi
Y.,
Sotudeh-Gharebagh
R.,
Talebizadeh A. Kinetic modelling of oxidative
coupling of methane over Mn/Na2WO4/SiO2
catalyst.//Fuel Processing Technology.
–
2009. 90(3). № 5.
–
p.403-410.
2.
Ji S., Xiao T., Li Sh., Chou L., Zhang B., Xu Ch.,
Hou R., York A.P.E., and Green M.L.H. Surface
WO
4
tetrahedron: this sence of the oxidative
coupling of methane over M
–
W
–
Mn/SiO
2
catalysts // Journal of Catalysis. 2003. Vol.
220.
Р
. 47-56.
3.
Тюняев
А
.
А
.,
Нипан
Г
.
Д
.,
Кольцова
Т
.
Н
.,
Локтев
А
.
С
.,
Кецко
В
.
А
.,
Дедов
А
.
Г
.,
Моисеев
И
.
И
.
Полиморфные
ОДМ
-
катализаторы
Mn/W/Na(K,Rb,Cs)/SiO
2
//
Журнал
неорганической химии. –
2009.
–
Т. 54. –
№
5.
–
С. 723
-726.
4.
Дедов А.Г., Локтев А.С., Тельпуховская Н.О.,
Пархоменко К.В., Геращенко М.В., Моисеев
И.И. Окислительная конденсация метана в
присуствии
лантан
-
цериевых
Volume 02 Issue 10-2022
33
American Journal Of Applied Science And Technology
(ISSN
–
2771-2745)
VOLUME
02
I
SSUE
10
Pages:
25-34
SJIF
I
MPACT
FACTOR
(2021:
5.
705
)
(2022:
5.
705
)
OCLC
–
1121105677
METADATA
IF
–
5.582
Publisher:
Oscar Publishing Services
Servi
катализаторов:
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Volume 02 Issue 10-2022
34
American Journal Of Applied Science And Technology
(ISSN
–
2771-2745)
VOLUME
02
I
SSUE
10
Pages:
25-34
SJIF
I
MPACT
FACTOR
(2021:
5.
705
)
(2022:
5.
705
)
OCLC
–
1121105677
METADATA
IF
–
5.582
Publisher:
Oscar Publishing Services
Servi
ахборотномаси.
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