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PUBLISHED DATE: - 30-12-2024
https://doi.org/10.37547/tajet/Volume06Issue12-21
PAGE NO.: - 206-221
STUDY OF THE KINETICS OF THE PROPANE-
BUTANE FRACTION PYROLYSIS PROCESS
Sanjar H. Saidqulov
Laboratory Assistant, Department Of Polymer Chemistry And Chemical
Technologies, Institute Of Biochemistry, Samarkand State University
Named After Sharof Rashidov, Samarkand, Uzbekistan
INTRODUCTION
In the global petrochemical industry, there is a
tendency to increase the demand for lower
alkenes. Thermal pyrolysis processes with "water
vapour" in tube furnaces are the main sources of
ethylene and propylene production [1-3], they are
used in various branches of the national economy
for the production of polyethene, polypropylene,
phenol, acetone, alcohols, varnishes, solvents, as
well as synthesis of other substances used as raw
materials as mediators to make.
Another urgent task in the production technology
of lower alkenes is the selection of raw materials
for the pyrolysis process.
To date, there are no industrial enterprises
producing lower alkenes by catalytic pyrolysis and
catalytic conversion of C3-C4 alkanes in
Uzbekistan. Lack of highly efficient catalysts is a
limiting factor[4-8]. In most cases, the proposed
catalysts for pyrolysis processes consist of various
individual and complex oxides, which are part of
zeolites and ceramics.
Research on catalytic pyrolysis of individual
hydrocarbons and technical mixtures made it
possible to form several laws that are important
for determining the mechanism of the process [9-
15]. It was found that hydrocarbons of the same
class (alkanes, alkenes) of these compounds do not
interact, and the composition of catalytic pyrolysis
products obeys the rule of additivity [16-23].
Aromatic hydrocarbons accelerate the process,
RESEARCH ARTICLE
Open Access
Abstract
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ethylene has no effect and propylene inhibits the
decomposition of alkanes [24-26]. The study of the
kinetics of catalytic pyrolysis of alkanes and their
mixtures showed that the order of the reaction is
one [27-31] or one and a half [32-36], depending
on whether the chains are broken by the
recombination of different or the same radicals.
The process of thermal pyrolysis of alkanes is
characterized by a first-order reaction [37-43].
The activation energy of catalytic pyrolysis of
alkanes varies widely depending on the type of
catalyst. For example, the pyrolysis activation
energy of various hydrocarbons in the presence of
potassium vanadate and stannate is in the range of
167-230 kJ/mol [44-48].
The laws of the catalytic pyrolysis process were
studied on the example of propane, n-butane,
ethylene, propylene and their mixtures [49-53].
Since there are many publications on catalysts for
the pyrolysis of hydrocarbons, we will only
consider catalysts for the pyrolysis of lower
alkanes [C
2
-C<]. The proposed catalysts are
composed of various individual and complex
oxides [54-58], ceramics [59-63], and cement [64-
68], which are part of zeolites.
Experimental part
In the calculations, it was assumed that the
dependence of the amount of moles of the
component on the peak surface is linear. The
composition of the products of the decomposition
reaction of the propane-butane mixture in the
absence of air and under the influence of heat and
breaking the C-C and C-H bonds was calculated
according to the following scheme:
a) The surface area (height) was recalculated to the
amount of substance according to the following
formula:
,
ef
i
ef
i
S
n
k
H
n
k
=
=
(1)
Here,
i
k
- which determines the sensitivity of the
detector to the same component.
b) then, the molar percentages were converted to
mass. To recalculate the mole fractions of the
components, they are multiplied by the
corresponding values of molecular masses:
i
i
i
m
M
=
(2)
c) according to the following equation the mass
concentration of the i-component was determined:
100%
i
i
i
i
m
m
=
(3)
g) the degree of change (X) was determined
according to the following formula:
int
int
prod
100%
Х
−
=
(4)
prod
- the total concentration of propane and
butane in the reaction products.
d) the selectivity of the component was found
according to the following equation:
100%
i
i
S
X
=
(5)
In addition to the composition of products in the
gas mixture, the formation of coke is the process of
breaking the S-S and S-N bonds in the propane-
butane mixture under the influence of high
temperature in an airless place was also conducted
in the reactor.
RESULTS AND DISCUSSION
Kinetic laws of thermal decomposition of propane-
butane hydrocarbon mixture. Decomposing the
propane-butane mixture in the absence of air at
high temperatures in the absence of air in a reactor
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designed for the process of breaking C-C and C-H
bonds has a significant effect on the process of
breaking C-C and C-H bonds. The surface of the
reactor designed to carry out the process is never
inert during the reaction. Therefore, in the pulse
and flow systems of the reactor surface designed
for the process, the propane-butane mixture is
broken under the influence of high temperature in
the absence of air, with the breaking of C-C and C-
H bonds as a result of decomposition at high
temperature without the presence of air in the
reactor designed for the process of breaking the C-
C and C-H bonds influence on the decomposition
process was studied.
From the data in Table 1 and Figures 1, and 2, it can
be seen that increasing the process temperature
from 500 to 800 °C helped to increase the yield of
ethylene and reached the maximum at 780 °C.
Table 1. Results of the decomposition reaction with the breaking of C-C and C-H bonds as a result
of decomposing a propane-butane mixture at high temperature without the presence of air
Contact
T, °С
Propane-
butane
fraction
conversion,
%
Productivity, wt.% in relation to transferred raw
materials
Selectivity
on C
2
H
4
, %
СН
4
С
2
Н
6
С
2
Н
4
С
3
Н
6
∑С
2
-
С
4
unsaturated
ethylenic series
hydrocarbons
An empty
reactor
designed to
carry out the
process
(
τ=6,6
s)
600
6.6
2.9
2.9
0.8
0
0.8
12.1
700
40.1
9.5
3.6
15.9
11.1
27.0
39.7
750
82.1
21.2
5.4
47.8
7.7
55.5
58.2
780
98.6
28.8
5.4
60.9
3.5
64.4
61.8
800
98.5
31.2
7.6
57.9
1.8
59.7
58.8
Reactor filled
with metal
fragments
(
τ=4,6
s)
600
6.6
2.9
2.9
0.8
0
0.8
12.1
700
40.1
9.5
3.6
15.9
11.1
27.0
39.7
750
82.1
21.2
5.4
47.8
7.7
55.5
58.2
780
98.6
28.8
5.4
60.9
3.5
64.4
61.8
800
98.5
31.2
7.6
57.9
1.8
59.7
58.8
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1
–
reactor designed for empty quartz process, 2
–
quartz reactor designed for process filled with metal
particles
Figure 1. Ethylene yield in the thermal decomposition of a propane-butane mixture in the absence
of air in a quartz reactor designed for the process in the absence and presence of metal fragments
1
–
an empty quartz reactor designed for the implementation of the process, 2
–
a quartz reactor designed
for the implementation of the process filled with metal particles
Figure 2. The yield of propylene in the thermal decomposition of a propane-butane mixture in the
absence of air in a reactor designed for the implementation of a quartz process in the absence of
metal fragments and in its presence
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Previously, the propane-butane mixture in the
quartz reactor designed for the process was
decomposed at high temperatures without the
presence of air in the reactor designed for the C-C
and C-H bond breaking under the influence of high
temperatures in the absence of air, it is believed
that it allows to exclude the effect. A detailed study
of the decomposition reaction leading to the
breaking of C-C and C-H bonds as a result of
decomposing a propane-propane-butane mixture
under the influence of high temperature in the
absence of air in a quartz reactor designed to carry
out the process of breaking C-C and C-H bonds at
high temperature in the absence of air, allowed us
to assume that it is carried out conditionally in the
following two directions through the chain free
radical mechanism in the gas phase:
As a sample reaction of the thermal transformation
of the propane-butane fraction in an air-free space
in a quartz reactor designed for a process filled
with chips of 0 = 0.3-0.5 mm (hereafter referred to
as "quartz") and as a result of decomposition at
high temperature in the reactor without the
presence of air under the influence of heat The
process of cleavage with the breaking off of C-C and
C-H bonds was studied. Table 2 shows the typical
experimental results of the decomposition
reaction with the breaking of C-C and C-H bonds as
a result of decomposing a propane-butane mixture
in a helium environment at high temperature in the
absence of air in a reactor designed for the process
of breaking C-C and C-H bonds at high temperature
without the presence of air.
Table 2. The results of the decomposition reaction of propane-butane mixture in a pulsed
system in a helium environment with the breaking of CC and CH bonds under the influence of
high temperature in the absence of air
Contact
T, °С
Propane-butane
fraction conversion,
%
Productivity, wt.% in relation to
transferred raw materials
СН
4
С
2
Н
6
С
2
Н
4
С
3
Н
6
An empty reactor
designed to carry out
the process (
τ=6,6
s)
600
43.0
13.7
0
20.0
9.3
700
69.6
22.9
0
37.5
9.2
750
81.2
28.0
0
45.5
7.7
780
87.7
34.9
0
50.9
1.9
800
87.2
37.5
1.1
47.6
1.0
A reactor designed for
the implementation of
the process filled with
metal fragments (
τ=9
.0
s)
600
43.5
23.4
2.6
17.5
0
700
64.6
31.5
4.1
29.0
0
750
82.3
37.4
5.2
39.7
0
780
94.7
41.1
5.3
46.3
2.0
800
95.7
41.9
5.5
46.5
1.8
A quartz reactor
designed for the
process (
τ=0,75
s)
600
31.2
6.9
1.0
12.7
10.6
700
50.0
11.2
3.0
22.1
13.7
750
78.5
37.9
3.0
27.9
9.7
780
89.5
43.0
4.0
34.4
8.1
800
98.8
38.3
5.0
48.0
7.5
From the data in Table 2, it follows that the yield
and ratio of the products of the decomposition
reaction of the propane-butane mixture under the
influence of high temperature in the absence of air
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by breaking the C-C and C-H bonds depends on
both the contact time and the volume of the contact
surface of the propane-butane fraction with quartz
(SiO2, SiO2-x (OH)x).
Based on the experimental data on the effect of
temperature on the yield of the products of the
decomposition reaction of the propane-butane
mixture under the influence of high temperature in
the absence of air, the activation energies of the
gross decomposition processes of the initially
saturated hydrocarbons and the formation of
reaction products are calculated (Table 3).
Table 3. Values of the activation energies of the gross processes of the consumption of initial
components (propane, butanes) and the assembly of their products in a reactor designed for the
process of breaking C-C and C-H bonds under the influence of high temperature in a helium
atmosphere in an air-free place of propane-butane mixture
Contact
τ, с
E
efa
, kJ/mol
СН
4
С
2
Н
4
С
3
Н
8
∑С
4
Н
10
An empty
reactor
6.6
62.6 ±3.9
85.1 ± 16.5
211.9 ± 9.2
302.9 ± 19.2
An empty
reactor
9.0
37.8 ±3.2
77.0 ±8.6
179.0 ± 14.9
287.6 ± 16.3
Quartz
0.75
35.9 ±2.7
109.4 ± 14.8
211.6 ±20.7
196.6 ±23.0
Before the physical adsorption of propane and
butane on quartz, it can be assumed that their
decomposition into radicals, and then the
decomposition process of the propane-butane
fraction in a reactor designed to break the S-S and
S-N bonds in a general airless space and under the
influence of heat, mainly develops on the surface of
quartz. The latter is consistent with the results of
other studies.
The temperature dependence of the propane-
butane fraction decomposition rate constant has
the following form:
An empty reactor designed to carry out the process
(τ=6.6, k=1.20∙1014∙exp(
-257.40/RT), c
–
1 (923-
1053 K);
An empty reactor designed to carry out the process
(τ=9.0 k=3.19∙1012∙exp(
-233.30/RT), c
–
1 (973-
1063 K);
The quartz reactor designe
d for the process (τ=6.6,
k=1.97∙1011∙exp(
-204.10/RT), c
–
1 (903-1083 K);
Thus, in the reactor designed for the process of
breaking the C-C and C-H bond under the influence
of high temperature of the propane-butane
mixture in an airless place at 500-800 °C, the
formation of coke in the presence and absence of
quartz in the helium environment is "suppressed"
by the initial hydrocarbons on the quartz surface is
shown to represent the catalytic decamp n.
The effect of the reactor material designed for the process in a reactor designed for the process of
breaking the S-S and S-N bonds under the influence of high temperature in an air-free space of a
propane-butane mixture in a flow system.
The results of the study are presented in Figures 3, and 4.
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Figure 3. Propylene yield during thermal decomposition of the propane-butane fraction in the
absence of air in quartz (1) and steel (2) reactors
Figure 4. Ethylene yield during thermal decomposition of the propane-butane fraction in the
absence of air in quartz (1) and steel (2) reactors
The amount of carbon deposits formed on the walls of the steel process reactor is five times higher than
that of the quartz process reactor (Table 4).
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Table 4. The selectivity of the decomposition reaction (T=850 ℃) in the reactor designed for the
process of breaking the C-C and C-H bond under the influence of high temperature in the absence
of air in the presence of "water vapour" in the flow system
Contact
С
2
Н
4
/СН
4
С
3
Н
6
/СН
4
С
2
Н
4
/С
3
Н
6
а*
cox,
weight %
A quartz reactor designed to
carry out the process
1.70
1.04
1.63
0.71
0.23
A steel reactor designed to carry
out the process
2.02
0.99
2.03
0.75
1.12
Note: a* is the percentage of consumption of propane and butanes involved in the targeted routes.
α =
𝑛
э
𝑛
э
+𝑛
п
,
𝑛
э
and
𝑛
п
-
- the amount of moles of
ethylene and propylene in the reaction mixture at
the exit from the reactor designed for the process.
Experimental results continue with the formation
of ethylene and propylene, in the absence of air and
under the influence of heat, and the propane-
butane mixture in the absence of air under the
influence of high-temperature C-C and C-H bond
allows to determine changes in the ratio of the
main directions of the decomposition reaction in
the reactor designed for the process of breaking
the.
The process of breaking the C-C and C-H bonds of
the propane-butane mixture in the absence of air
under the influence of high temperature was also
carried out in a quartz reactor designed for the
implementation of the process filled with quartz-
quartz pieces Ø = 0.3-0.5 mm (Table 5).
The experimental results presented in Table 5
show that during the decomposition reaction in
quartz in the absence of air and under the influence
of heat and propane-butane mixture under the
influence of high temperature in the absence of air,
the contact time increases, the conversion of raw
materials and the yield of ethylene increase at the
same temperature. , the propylene yield passes
through a maximum (~820 ℃).
Table 5. Results of the decomposition reaction of the propane-butane mixture in a flow system
with the presence of "water vapour" under the influence of high temperature in the absence of
air with the breaking of C-C and C-H bonds
Contact
T,
°С
Propane-
butane
fraction
conversion,
%
Productivity, wt.% in relation to transferred
raw materials
Selectivity
on
С
2
Н
4
, %
СН
4
С
2
Н
6
С
2
Н
4
С
3
Н
6
∑С
2
-
С
4
unsaturated
ethylenic
series
hydrocarbons
An empty
reactor
designed to
730
10.5
2.7
1.5
3.3
3.0
6.3
31.4
770
25.2
4.2
3.7
6.6
10.7
17.3
26.2
820
53.4
10.4
3.8
22.6
16.6
39.2
42.3
840
63.3
13.5
4.8
25.6
19.4
45.0
40.4
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carry out the
process (
τ
=1.5 s)
880
87.5
20.7
5.2
43.5
18.1
61.6
49.7
Quartz reactor
designed for
process
implementation
(
τ
=0.7 s)
730
10.7
1.9
0.9
2.6
5.3
7.9
24.3
770
31.0
5.9
3.2
8.8
13.1
21.9
28.4
820
79.4
19.6
5.3
29.4
25.1
54.5
37.0
850
92.6
25.2
5.7
40.1
21.6
61.7
43.3
870
97.9
32.3
7.4
46.8
12.4
59.2
47.8
A quartz reactor
(
τ
=6.6 s)
designed for the
implementation
of the process
730
23.9
4.2
1.8
6.3
11.6
17.9
26.4
770
48.5
9.9
3.1
15.4
20.1
35.5
31.8
825
85.4
19.7
5.6
39.4
20.7
60.1
46.1
845
97.7
30.1
7.0
46.6
14.0
60.6
47.7
The difference in ethylene production can be
explained by the presence of a catalytic effect, as
well as the fact that the presence of quartz
significantly increases the contact surface
(heterogeneous factor S/V (S is the internal surface
area of the reactor designed for the
implementation of the process, V is the volume of
the reactor designed for the implementation of the
process) from 10 times increases more). Based on
the radical chain mechanism, it can be assumed
that the rate of heterogeneous decomposition of
saturated hydrocarbons increases with increasing
S/V at low temperatures and the rate of
heterogeneous chain termination increases at high
temperatures.
Based on the obtained results, activation energies
were determined (Table 6). It should be noted that
these activation energies are effective quantities
associated with the entire process (decomposition
of propane and butanes, formation of methane and
ethylene). Calculation of the effective activation
energy, on the one hand, the process of breaking
the S-S and S-N bond under the influence of high
temperature in the airless place of propane-butane
mixture was also carried out in a quartz reactor
filled with quartz-quartz fragments Ø = 0.3-0.5 mm
ng homogeneous- allows to clarify the
heterogeneous mechanism, on the other hand, to
obtain comparative information about the
efficiency of catalytic systems.
Table 6. Values of the activation energies of the gross processes of the consumption of the main
initial components (propane, butanes) and the assembly of their products in the decomposition
reaction with the breaking of C-C and C-H bonds as a result of the decomposition of the propane-
butane mixture at high temperature in the flow system with the presence of "water vapour"
Contact
t, s
E
efa
, kJ/mol
СН
4
С
2
Н
4
С
3
Н
8
∑С
4
Н
10
An empty reactor
1.5
147.8 ±5.5
140.3 ± 4.6
168.5 ±6.1
140.4 ± 4.2
An empty reactor
0.7
175.9 ±7.0
185.7 ±6.2
230.6 ± 7.2
273.4 ± 9.4
Quartz
6.6
139.3 ± 4.2
172.5 ±3.6
178.9 ±3.9
205.9 ±6.1
The temperature dependence of the propane-
butane fraction decomposition rate constant is
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expressed by the following equations:
An empty reactor designed to carry out the process
(t=1.5s)k=1.20∙1014∙exp(
-257.40/RT), c
–
1 (923-
1053 K);
An empty reactor designed to carry out the process
(t=0.7s)k=3.19∙1012∙exp(
-233.30/RT), c
–
1 (973-
1063 K);
Quartz reactor designed for the process
implementation
(t=6.6s)k=1.97∙1011∙exp(
-
204.10/RT), c
–
1 (903-1083 K);
Kinetic laws of the decomposition reaction in a
reactor designed to break the S-S and S-N bonds
under the influence of high temperature in a
vacuum of propane-butane mixture. From the
results of the kinetic study, it follows that the
decomposition reaction of lower molecular
saturated hydrocarbons at atmospheric pressure,
at moderate temperatures (up to 750 °C) in airless
space and under the influence of heat proceeds to
the first order, since the values of ln(1/1-X)
increased linearly with increasing X ( Figure 5).
Figure 5. In an empty quartz reactor at T=700°С, the propane
-butane mixture is decomposed by
breaking the C-C and C-H bonds under the influence of high temperature in an airless
place.ln(1/1-X) as a function of contact time
Based on the dependence of lnk and 1/T in
Arrhenius coordinates (Figs. 6, 7), CC and The
dependence of the effective activation energies of
the decomposition reaction with the breaking of C-
H bonds and their decomposition rate constant
was determined:
Propane k=8.81∙1015∙exp(
-243.70/RT), c
–
1 (913-
1013 K);
Butane k=2.00∙1014∙exp(
-268.60/RT), c
–
1 (973-
1013 K).
Figure 6. Semi-logarithmic anamorphism of temperature dependences of effective rate constants
(c
–
1) of propane decomposition reactions, coupled reactions of ethylene and methane formation
in an empty reactor designed to implement the process
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Figure 7. Semi-logarithmic anamorphism of effective rate constants (c
–
1) of temperature
dependences of n-butane decomposition reactions, adjacent reactions of ethylene and methane
formation in an empty reactor designed to implement the process
Table 7. Values of the activation energies of the gross processes of the consumption of the main
initial components (propane, butanes) and the accumulation of their products in the
decomposition reaction with the breaking of C-C and C-H bonds in an empty quartz reactor
Hydrocarbon
t, s
E
efa
, kJ/mol
SN4
S2N4
S3N8
∑S4N10
Propane
6.6
185.7 ±6.5
205.5 ± 10.0
243.7 ± 11.4
-
Bhutan
6.6
132.5 ±5.6
176.1 ± 8.1
-
268.6 ± 13.7
The values of activation energies obtained from
experimental data were compared with those
found theoretically using reference values of
binding energies based on the assumption of
transition state formation in quartz.
CONCLUSIONS
Thus, it was shown that the catalytic
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decomposition of primary hydrocarbons on the
surface of quartz in the presence and absence of
quartz in a reactor designed for the cleavage of C-C
and C-H bonds in the absence of air at 500-800 ° C
represents the formation of coke in the presence
and absence of quartz in a helium environment.
Based on the relationship between lnk and 1/T in
Arrhenius coordinates, the relationship between
the effective activation energies of the
decomposition reaction with the cleavage of C-C
and C-H bonds and their decomposition rate
constants were determined as a result of the
decomposition of propane-butane mixtures in a
reactor designed for the cleavage of C-C and C-H
bonds in the absence of air at high temperatures.
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