American Journal of Applied Science and Technology
26
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VOLUME
Vol.05 Issue 05 2025
PAGE NO.
26-32
10.37547/ajast/Volume05Issue05-07
Evaluation of The Efficiency of Selected Catalysts for
The Pyrolysis of a Propane
–
Butane Fraction
Sanjar H. Saidqulov
Laboratory assistant, Department of Polymer Chemistry and Chemical Technologies, Institute of Biochemistry, Samarkand State
University named after Sharof Rashidov, Samarkand, Uzbekistan
Normurot I. Fayzullayev
Doctor of Chemical Sciences, Professor, Samarkand State University named after Sharof Rashidov, Institute of Biochemistry,
Department of Polymer Chemistry and Chemical Technologies, Samarkand, Uzbekistan
Hayitali N. Ibodullayev
Student, Institute of Biochemistry, Samarkand State University named after Sharof Rashidov, Samarkand, Uzbekistan
Received:
13 March 2025;
Accepted:
09 April 2025;
Published:
11 May 2025
Abstract:
This study evaluates the efficiency of selected catalysts for the pyrolysis of a propane
–
butane fraction
under inert, oxygen-free conditions. Experiments were conducted in both pulse and flow reactors within a
temperature range of 650
–860 °C. Catalyst perf
ormance was assessed based on conversion and selectivity. In a
quartz reactor, thermal cracking led to high yields of unsaturated hydrocarbons, especially ethylene and propylene,
with ethylene selectivity reaching 55% at 730 °C. Flow reactors with Zn
-, Cu-, Mn-, and Fe-based coatings showed
that the Zn-coated system provided the highest olefin yield (62.2 wt.%) and minimal coke formation (0.24%).
Activation energy analysis indicated that Zn required less energy (150
–200 kJ/mol), supporting a radical reactio
n
mechanism. The catalytic activity followed the order: Zn > Cu > Mn > Fe. The enhanced performance of Zn is
attributed to its low oxidation state and hydrogenation capability, which suppresses coke formation. These results
demonstrate the critical role of catalyst material and reaction environment in maximising olefin production during
propane
–
butane pyrolysis.
Keywords:
Propane
–
butane, catalytic activity, ethylene, coke, quartz reactor.
Introduction:
Currently, the efficient processing of hydrocarbon
feedstocks is of critical importance in both the
industrial and energy sectors. Pyrolysis of propane
–
butane
fractions
under
oxygen-free,
high-
temperature conditions enables the production of
valuable compounds such as ethylene, propylene,
butadiene, and aromatic hydrocarbons. This process
plays a key role not only in the petrochemical industry
but also in the manufacturing of polymers, fuels, and
organic intermediates [1
–
3].
Globally, various catalysts are being developed to
optimise pyrolysis processes and reduce energy
consumption. Catalysts based on nickel, chromium,
aluminosilicates, and zinc have been widely applied to
improve
process
efficiency.
These
catalysts
contribute to lowering the required reaction
temperature, increasing the yield of target products,
and suppressing undesired side reactions [4
–
8].
In Uzbekistan, research is also being conducted in this
direction. The Bukhara Institute of Engineering and
Technology is engaged in improving pyrolysis
technologies for liquid petroleum products and
performing calculations for key processing equipment
[9
–
15]. In addition, studies are being carried out in
the field of petroleum and gas refining technologies,
focusing on evaluating catalyst performance and
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
implementing innovative technological solutions.
METHODS
Two types of reactor systems were used in this study
to carry out the pyrolysis of a propane
–
butane
mixture: a pulse microreactor and a flow reactor. All
experiments were conducted in an inert (oxygen-
free) atmosphere within the temperature range of
650
–860 °C.
Reaction
conditions
such
as
temperature, residence time, and type of coating
were varied to assess their impact on process
efficiency.
In the initial stage, thermal decomposition of propane
and butane was studied in a blank quartz tube using
the pulse reactor, without any catalytic influence.
Under these conditions, only thermal cracking
occurred due to the high temperature. The results
showed that increasing the temperature up
to 730 °C
significantly improved the conversion of the
propane
–
butane fraction and the selectivity toward
olefins
—particularly ethylene (C₂H₄) and propylene
(C₃H₆), with selectivity reaching up to 55%.
In the next stage, experiments were conducted in a
flow reactor equipped with wall coatings of different
metals: Zn, Cu, Mn, and Fe. Each metal coating was
evaluated based on overall cracking efficiency,
combined olefin yield (C₂H₄ + C₃H₆), coke formation,
and activation energy characteristics.
According to the experimental results, the Zn-coated
reactor achieved the highest olefin yield (62.2 wt.%),
the lowest coke formation (0.24%), and the lowest
activation energy (150
–200 kJ/mol). This behaviour is
attributed to the low oxidation state and high
hydrogenation ability of the Zn surface, which helps
suppress coke formation. The overall catalytic
performance and inhibitory effect of the metal
coatings followed the order: Zn > Cu > Mn > Fe.
RESULTS AND DISCUSSION
The kinetic behaviour of thermal decomposition of a
propane
–
butane mixture under oxygen-free and
high-temperature conditions was studied with
respect to the reactor wall material. The efficiency of
high-temperature pyrolysis in an inert environment is
largely influenced by the characteristics of the
selected catalyst. Catalyst performance is primarily
assessed by its catalytic activity, i.e., the amount of
feedstock converted per unit time, and its selectivity,
i.e., the ability to produce target products such as
ethylene, propylene, and other unsaturated
C₂–C₄
hydrocarbons.
The following criteria are commonly used to evaluate
catalytic activity:
•
Conversion rate (X)
–
the percentage of the
hydrocarbon
feedstock
that
undergoes
transformation relative to the initial amount;
•
Rate constant (k)
–
the kinetic parameter
characterising the speed of the reaction;
•
Yield (Y)
–
the amount of target product (e.g.,
g/m³) such as ethylene or propylene produced;
•
Selectivity (S)
–
the ratio of target product
yield to the total amount of products formed.
To determine these parameters, the pulse
microreactor method is widely used. In this approach,
a short pulse of the propane
–
butane mixture is
introduced into a preheated reactor, and the
decomposition results are analysed. This method
enables rapid and reliable evaluation of the relative
activity and selectivity of catalysts.
During pulse reactions, the propane
–
butane mixture
is introduced at a defined flow rate through a
specially designed reactor using a carrier gas. The
temperature within the catalyst bed is raised to 500
–
800 °C, allowing the feedstock to undergo pyrolysis.
The reaction products are separated and quantified
using gas chromatography at the reactor outlet.
Gas chromatography allows identification of the
following components:
•
Unsaturated
hydrocarbons:
ethylene,
propylene, butenes;
•
Saturated hydrocarbons: ethane, propane,
butane;
•
By-products: methane, hydrogen, coke, and
others.
An essential aspect of catalyst performance is its
operational stability, or its ability to retain catalytic
properties over an extended period. This parameter
is usually assessed through multi-day experiments. A
decline in catalyst activity over time is typically
attributed to deactivation, fouling of active sites, or
coking. In such cases, a layer of graphite-like carbon
may form inside the reactor, blocking the active
surface of the catalyst.
Optimal Conditions and Coke Formation
To maximise the yield of the target product
—
ethylene
—
while minimising coke formation, it is
essential to determine the optimal reaction
temperature, residence time, and carrier gas flow
rate. According to experimental results:
•
At 600
–700 °C, propane and butane undergo
high conversion rates;
•
Above 700 °C, selectivity ten
ds to decrease,
and coke formation increases.
•
A residence time of 2
–
5 seconds results in the
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
highest ethylene yields.
In addition, the regeneration capacity of the catalyst
was evaluated. A catalyst that can restore its activity
after several operating cycles is considered reliable
and effective.
Influence of Reactor Material on Thermal Cracking
During the pyrolysis of a propane
–
butane mixture at
high temperatures in an inert atmosphere, the
chemical and physical properties of the reactor
material play a critical role in determining the
reaction efficiency. Specifically, the interaction
between the reactor walls or internal inserts and the
reaction medium
—
i.e., heterogeneous surface
effects
—
can influence the mechanism of thermal
transformation and the selectivity of the products.
Two reactor configurations were compared
experimentally:
1.
Blank quartz reactor, made entirely of quartz
glass without any internal filler;
2.
Quartz reactor filled with metal (steel)
inserts, where pieces of industrial-grade steel were
placed inside the reactor.
Experiments conducted within the temperature
range of 500
–800 °C showed that the conversion of
C₁–C₄
hydrocarbons
increased
with
rising
temperature. For instance, at 750 °C:
•
The blank quartz reactor exhibited a
conversion rate of 82.1%;
•
The steel-filled reactor showed a slightly
lower conversion rate of 78.5%.
Significant differences were also observed in the yield
of unsaturated ethylene series hydrocarbons (C₂–C₃
fractions):
•
In the quartz reactor, the total mass fraction
reached 55.5 wt.%;
•
In the steel-filled reactor, this figure
decreased to 43.5 wt.%.
These results highlight the influence of reactor
materials on catalytic activity and reaction pathways.
Construction materials should not induce unintended
catalytic effects. The quartz reactor, being chemically
inert, serves as a neutral medium, ensuring high
selectivity and reactivity.
Activation Energy Analysis
In experiments carried out in a quartz reactor without
any catalyst, the calculated effective activation
energies for the thermal decomposition of propane
and butane hydrocarbons were as follows:
•
Propane: ~197 kJ/mol
•
Butane: ~303 kJ/mol
These values, when compared to the C
–
C bond
dissociation energy and the heat of physical sorption
on silica gel (~326 k
J/mol), suggest that both propane
and butane molecules are relatively prone to thermal
transformation under the given conditions.
Effect of Water in the Reaction Medium
The presence of water vapour in the reaction
environment was identified as one of the factors
reducing the activity of quartz materials. This effect is
primarily attributed to chemisorption of water on the
quartz surface, which blocks active surface sites and
decreases the overall activity of the reactor medium
intended for hydrocarbon conversion.
Kinetics of Individual Saturated Hydrocarbons
(Propane and Butane)
Studying the thermal decomposition kinetics of the
individual components of the propane
–
butane
feedstock
—namely propane (C₃H₈) and n
-butane
(C₄H₁₀)—
is essential for understanding their
respective reaction mechanisms and optimising
reactor parameters.
In this section, the temperature-dependent
behaviour of propane and butane was examined
separately. Experiments were conducted in a blank
quartz reactor to eliminate heterogeneous surface
effects and ensure an inert environment. The
objective was to assess the individual kinetic
behaviour of each component in the mixture by
isolating their contributions.
Experimental Conditions and Methodology
The pyrolysis of propane and n-butane was carried
out at high temperatures (650
–730 °C) under oxygen
-
free conditions. The reaction products were identified
and quantified using gas chromatography, with both
qualitative and quantitative analyses performed.
Table 1 presents the major products formed at
various temperatures and their corresponding
concentrations (in mass %):
Table 1. Thermal Cracking Results of Propane and n-Butane (in a Blank Quartz Reactor)
Hydrocarbons
(wt.%)
Temperat
ure (°C)
650
680
700
730
650
680
700
C₃H₈
н
-
C₄H₁₀
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
CH₄
2.0
3.4
9.3
18.8
3.8
7.8
15.9
C₂H₆
0
0.2
0.7
2.1
0.2
0.6
1.2
C₂H₄
2.9
6.6
15.8
40.4
6.7
17.1
34.6
C₃H₆
2.5
4.8
15.1
11.5
8.4
17.0
18.2
Unsaturated
C₂–C₃
5.4
11.4
30.9
51.9
15.1
34.7
52.8
Conversion (%)
10.3
15.0
40.9
72.8
19.1
43.1
69.9
C
₂
H
₄
selectivity (%)
28.2
44.0
38.6
55.5
35.1
41.1
49.5
Conversion, Product Distribution, and Reaction
Selectivity
Conversion
: As the reaction temperature increased,
the conversion rates of both propane and butane
significantly rose. At 730 °C, propane reached a
conversion of 72.8%, while n-butane achieved as high
as 97.8%, indicating the greater susceptibility of the
n-butane molecule to thermal decomposition.
Formation of Unsaturated Hydrocarbons: Both
propane and butane, at 700
–730 °C, led to the
formation of unsaturated hydrocarbons such as
ethylene (C₂H₄) and propylene (C₃H₆). The mass
fraction of unsaturated hydrocarbons from butane
reached 68.2 wt.%, which is higher than that from
propane (51.9 wt.%).
Selectivity
: The selectivity toward C₂H₄ in both cases
ranged between 40% and 55%, peaking at 730 °C.
While butane’s C₂H₄ selectivity was slightly lower
(51.4%) than propane’s, its hig
her conversion rate
compensated for this difference.
These experimental results clearly demonstrate that
the pyrolysis of a propane
–
butane mixture under
high-temperature
and
oxygen-free
conditions
proceeds via a radical chain mechanism. The process
exhibits both homogeneous and heterogeneous
characteristics, where the reactor environment,
especially the material of the reactor walls,
significantly affects the kinetics and reaction
mechanisms.
Key Observations:
•
Influence of Reactor Wall Material: In an inert
quartz reactor, the reaction occurs predominantly in
the gas phase, minimising the formation of
undesirable products such as polymers, soot, and
coke.
•
Reduced Coke Formation: In pulse-mode
quartz reactors, radical fragments are rapidly swept
out by the carrier gas, lowering the probability of
olefin polymerisation and coke deposition.
•
Product Selectivity: Quartz reactors enabled
the efficient formation of lower unsaturated
hydrocarbons (C₂–C₄ olefins) with high yield and
selectivity from both propane and butane.
Table 2. Pyrolysis results of a propane
–butane mixture (τ = 1.5 s) in a flow system under oxygen
-free conditions
using selected catalysts at high temperature.
Interaction
Т, °С
Propane-
butane
hydrocarb
on mixture
conversion
, %
Productivity, wt.% in relation to transferred raw
materials
Selectiv
ity on
С
2
Н
4
, %
СН
4
С
2
Н
6
С
2
Н
4
С
3
Н
6
∑С
2
-
С
4
molecularly
unsaturated
ethylene series
hydrocarbons
Zn-retaining
coating
740
13.4
1.8
1.6
3.8
6.2
10.0
28.4
760
20.9
3.0
1.5
6.5
9.9
16.4
31.1
775
27.9
4.9
1.0
10.2
11.8
22.0
36.6
800
28.9
4.6
0.9
10.9
12.5
23.4
37.7
820
42.9
8.7
1.2
17.4
15.6
33.0
40.6
845
69.9
15.2
1.5
33.8
19.4
53.2
48.4
855
79.5
14.8
2.5
46.2
16.0
62.2
58.1
Cu-retaining
coating
730
8.7
1.5
0
2.8
4.4
7.2
32.2
760
17.7
3.9
0.6
6.8
6.4
13.2
38.4
785
34.3
7.4
2.5
12.4
12.0
24.4
36.2
800
40.3
8.7
2.4
15.1
14.1
29.2
37.5
840
68.4
17.0
3.5
29.7
18.2
47.9
43.4
855
81.4
21.8
4.9
36.9
17.8
54.7
45.3
750
18.6
2.1
0.3
6.0
10.2
16.2
32.3
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
Mn-sparing
coating
770
28.2
4.6
0.4
8.9
14.3
23.2
31.6
790
37.9
7.2
1.2
13.0
16.5
29.5
34.3
810
48.2
10.5
2.0
18.6
17.1
35.7
38.6
830
57.7
11.6
3.5
24.6
18.0
42.6
42.6
850
74.3
17.6
4.8
31.8
20.1
51.9
42.8
Fe-retaining
coating
730
5.1
0.5
2.1
0.7
1.8
2.5
13.7
760
11.0
1.5
2.1
2.9
4.5
7.4
26.4
790
17.0
3.2
2.3
4.7
6.8
11.5
27.6
810
29.9
5.3
2.5
9.7
12.4
22.1
32.4
845
45.6
9.4
3.1
17.3
15.8
33.1
37.9
860
68.7
15.5
3.7
29.5
20.0
49.5
42.9
Uncoated steel
reactor
730
8.6
1.6
0.5
2.7
3.8
6.5
31.4
750
21.9
4.1
1.5
7.1
9.2
16.3
32.4
765
24.5
4.9
2.0
8.4
9.2
17.6
34.3
790
39.7
8.0
3.9
14.3
13.5
27.8
36.0
830
63.9
13.2
7.0
28.2
15.5
43.7
44.1
850
76.0
17.1
7.4
34.5
17.0
51.5
45.4
Influence of Catalyst Coating Composition and
Selectivity Analysis
The results above indicate that the nature of the
metal in the catalytic film coating has a significant
impact on the overall conversion and the efficiency of
target
product
formation,
even
without
fundamentally altering the reaction mechanism. The
highest yield of light unsaturated hydrocarbons in the
C₂–C₃ range (62.2 wt.%), along with the lowest coke
formation rate, was obtained using a zinc-based
coating during the high-temperature pyrolysis of a
propane
–
butane
mixture
under
oxygen-free
conditions (see Tables 1 and 2).
Additionally, coatings containing Cu and Zn
demonstrated increasing propylene yields with rising
temperature, followed by a decline due to secondary
reactions of the formed products.
As shown in Table 2, the Zn-coated reactor exhibited
a higher conversion efficiency for propane and
butane into ethylene (conversion factor = 0.81)
compared to thermal pyrolysis (conversion factor =
0.75), indicating the catalytic promotion effect of Zn.
The overall yield of ethylene and propylene was also
higher in the Zn-coated system relative to non-
catalytic thermal cracking.
The lowest amount of coke deposition was recorded
for the Zn-containing coating, comparable to results
obtained in an inert quartz reactor during the
pyrolysis of a propane
–
butane fraction (see Table 3).
Table 3. Selectivity of propane
–
butane hydrocarbon mixture pyrolysis in a flow reactor under oxygen-free
conditions at T = 850 °C.
Interaction
С
2
Н
4
/СН
4
С
3
Н
6
/СН
4
С
2
Н
4
/С
3
Н
6
а*
Coke,
wt.%
The steel reactor is
unlined
2.02
0.99
2.03
0.75
1.12
A steel jacketed reactor designed to decompose the propane and butane
mixture fraction by heating it in a vacuum and at high temperature
Zn-retaining coating
3.12
1.08
2.89
0.81
0.24
Cu-retaining coating
1.69
0.82
2.07
0.76
1.20
Mn-sparing coating
1.81
1.14
1.58
0.70
1.25
Fe-sparing coating
1.90
1.68
1.48
0.70
1.05
Note and Selectivity Coefficient α*:
The coefficient
α*
represents the fractional consumption of propane
and butane involved in target-oriented reaction pathways (3.1
–
3.4). It is defined by the equation:
e
e
p
n
n
n
=
+
Where:
•
e
n
= number of moles of ethylene in the reactor outlet mixture,
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
•
p
n
= number of moles of propylene in the reactor outlet mixture.
As seen from Table 3, a key factor influencing catalytic
activity is the nature of the metal cation in the film
coating.
Based on the combined ethylene and propylene yield,
the catalytic activity of metal-containing coatings
follows the trend:
Zn > Cu > Mn > Fe
The same sequence is observed when considering the
inhibitory effect on coke formation.
The superior catalytic activity of the Zn-containing
coating is most likely attributed to zinc's low oxidation
potential and high hydrogenation ability, which
reduces the formation of polycondensation products.
In contrast, other metal oxides (e.g., CuO, MnO₂,
Fe₂O₃) may accelerate hydrocarbon aromatisation,
leading to increased coke accumulation on the
catalytic surface.
Analysis of Kinetic Parameters Based on Table 4
To gain deeper insight into the reaction mechanisms
involved in the high-temperature pyrolysis of a
propane
–
butane hydrocarbon mixture under inert
(oxygen-free) conditions, the activation energy of the
gross process was calculated.
Experiments were performed using reactor walls
coated with different metallic films (Zn, Cu, Mn, Fe),
and the calculated kinetic data are summarised in
Table 4.
Table 4. Activation energies for the pyrolysis of a propane
–butane hydrocarbon mixture (τ = 1.5 s)
Reactor coating
CH₄ (kJ
/mol)
С₂Н₄ (kJ/mol)
С₂Н₄ (kJ/mol)
∑C₄H₁₀ (kJ/mol)
Uncoated (steel)
130.0 ± 3.6
164.0 ± 6.5
205.5 ± 8.2
175.9 ± 6.2
Zn-coated
154.8 ± 4.2
149.9 ± 4.2
150.0 ± 5.3
200.8 ± 6.1
Cu-coated
164.8 ± 6.1
158.3 ± 4.9
237.3 ± 8.4
200.1 ± 7.8
Mn-coated
173.7 ± 5.6
154.5 ± 4.7
178.2 ± 8.8
172.8 ± 6.3
Fe-coated
179.2 ± 6.7
188.2 ± 7.1
198.0 ± 7.8
175.9 ± 7.9
Analysis and explanation of activation energies
The activation energies (Eₐ
-eff) presented in this table
serve to study the effect of various metal coatings on
the reaction rate. It is apparent that metal elements
have a heterogeneous effect on the homogeneous-
gas phase processes inside the reactor. This effect is
characterised by a high energy requirement,
especially for Cu and Fe coatings, which indicates a
strong inhibition of the reaction.
The lower Eₐ
-eff values achieved with Zn coatings are
due to the property of this metal to facilitate radical
formation and dissociation reactions. At the same
time, Mn coatings also provide moderate activity and
form a stable reaction environment.
CONCLUSION
Based on the conducted research, the following
conclusions were drawn:
1.
The thermal pyrolysis of a propane
–
butane
mixture at elevated temperatures (650
–860 °C) under
inert conditions proceeds via a radical chain
mechanism. In this process, the reactor material and
its internal coating play a critical role.
2.
Experiments conducted in an empty quartz
reactor
demonstrated
high
conversion
and
selectivity. The inertness of the reactor wall material
positively influenced the reaction efficiency.
3.
When steel reactors were coated with Zn, Cu,
Mn, and Fe, the catalytic activity and selectivity
significantly varied. The highest total yield of ethylene
and propylene (62.2 wt.%) was observed with the Zn-
containing coating.
4.
The Zn coating exhibited the lowest
activation energies (150.0 kJ/mol for propane),
enabling efficient control over the formation of target
products. Additionally, it demonstrated the lowest
coke formation (0.24%), highlighting its effectiveness.
5.
Maximum yield of ethylene and propylene
was achieved within the temperature range of 700
–
730 °C and a residence time of 1.5–
5 seconds.
Temperatures excee
ding 750 °C led to reduced
selectivity and an increased likelihood of coke
formation.
6.
The long-term operational stability and
regeneration potential of the catalysts were also
evaluated. Zn and Cu coatings retained their catalytic
activity well over multiple cycles.
In summary, reactors coated with Zn-based films
showed high activity, selectivity, and minimal coke
deposition during the pyrolysis of propane
–
butane
mixtures. These results support their application as a
promising technological solution for the efficient
production of olefins.
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American Journal of Applied Science and Technology (ISSN: 2771-2745)
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