MODELING AND APPROVAL OF METHANE NANOCARBON REACTOR

МОДЕЛИРОВАНИЕ И УТВЕРЖДЕНИЕ МЕТАНОВОГО НАНОУГЛЕРОДНОГО РЕАКТОРА
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Kholmirzayeva K., Fayzullayev N. MODELING AND APPROVAL OF METHANE NANOCARBON REACTOR // Universum: химия и биология : электрон. научн. журн. 2022. 4(94). URL: https://7universum.com/ru/nature/archive/item/13347 (дата обращения: 03.03.2024).
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DOI - 10.32743/UniChem.2022.94.4.13347

 

ABSTRACT

The process of nanocarbon of methane from methane was carried out in the presence of two types of catalysts: cat №1 and cat №2. The essence of the method is the interaction of nitrate mixtures of metals included in the catalyst and the organic matter in the air at temperatures ≥500 ℃. The reaction is followed by the formation of finely dispersed oxides of metals. It allows calculating the concentration of system components not only at the outlet of the apparatus but also along the length of the reactor. We calculated the average reaction rate in the presence of this (Fe2(MoO4)3*MoO3) catalyst 25 min after the start of the experiment. The area of decrease in the rate of formation of carbon layers in the catalyst has no experimental curves when the gas velocity is subsequently increased. This can be explained by the much higher activity of cat №2, which provides much higher rates of reactions in the catalyst. As a result, the methane supplied to the surface of the catalyst manages to interact with it before methane escapes with a stream of the initial gas mixture. The process should be carried out at linear velocities of not less than 25 cm/min of the initial gas mixture flow. Subsequent studies were performed on methane at a linear velocity of 35 cm/min. The results of the study of the effect of temperature on the rate of nanocarbon synthesis showed that cat №2 differs from cat №1 in the catalyst. The application of cat №2 at lower temperatures allows the production of nanocarbon with a much higher specific yield. The kinetic curves of the time dependence of the change in the specific amount of carbon in the catalyst do not have an induction period at all. The results of the experimental measurements are shown in Figure 4. The diameter of the reactor is 54 mm, and the length of the heated part is 300 mm. The process temperature did not change and was 650 ℃. The linear velocity of the gas supply (or its flow rate), as well as the catalyst flow rate, were varied. Thus, real experiments were repeated using computer technology. In determining the optimal conditions for the synthesis of methane in the catalytic pyrolysis reactor, it is important to determine the acceptance criteria and control parameters. The peculiarity of the nanocarbon production process is that the catalyst is consumed during the process. That is, the catalyst consumption is high with the low productivity of the nanocarbon, which does not allow the product to achieve a low cost. That is, the catalyst consumption is high with the low productivity of the nanocarbon, which does not allow the product to achieve a low cost. Process temperature and catalyst flow rate were taken as control parameters. In the calculations, the linear velocity of the gas phase was assumed to be 35 cm/min.

АННОТАЦИЯ

Процесс получения наноуглерода метана из метана осуществлялся в присутствии двух типов катализаторов: cat №1 и cat №2. Суть метода заключается во взаимодействии нитратных смесей металлов, входящих в состав катализатора, и органического вещества в воздухе при температурах ≥500 ℃. За реакцией следует образование мелкодисперсных оксидов металлов. Это позволяет рассчитать концентрацию компонентов системы не только на выходе из аппарата, но и по длине реактора. Мы рассчитали среднюю скорость реакции в присутствии этого катализатора (Fe2(MoO4)3*MoO3) через 25 мин после начала эксперимента. Область уменьшения скорости образования углеродных слоев в катализаторе не имеет экспериментальных кривых при последующем увеличении скорости газа. Это можно объяснить гораздо более высокой активностью cat №2, которая обеспечивает гораздо более высокие скорости реакций в катализаторе. В результате метан, подаваемый на поверхность катализатора, успевает взаимодействовать с ним до того, как метан выходит с потоком исходной газовой смеси. Процесс должен осуществляться при линейных скоростях потока исходной газовой смеси не менее 25 см/мин. Последующие исследования были проведены на метане с линейной скоростью 35 см/мин. Результаты исследования влияния температуры на скорость синтеза наноуглерода показали, что cat №2 отличается от cat №1 катализатором. Применение cat №2 при более низких температурах позволяет получать наноуглерод с гораздо более высоким удельным выходом. Кинетические кривые зависимости изменения удельного количества углерода в катализаторе от времени вообще не имеют индукционного периода. Результаты экспериментальных измерений показаны на рисунке 4. Диаметр реактора составляет 54 мм, а длина нагреваемой части - 300 мм. Температура процесса не изменилась и составила 650 ℃. Линейная скорость подачи газа (или его расход), а также расход катализатора варьировались. Таким образом, реальные эксперименты были повторены с использованием компьютерных технологий. При определении оптимальных условий синтеза метана в реакторе каталитического пиролиза важно определить критерии приемлемости и параметры контроля. Особенностью процесса производства наноуглерода является то, что в процессе расходуется катализатор. То есть расход катализатора высок при низкой производительности наноуглерода, что не позволяет продукту достичь низкой стоимости. То есть расход катализатора высок при низкой производительности наноуглерода, что не позволяет продукту достичь низкой стоимости. В качестве контрольных параметров были взяты температура процесса и расход катализатора. В расчетах линейная скорость газовой фазы принималась равной 35 см/мин.

 

Keywords: reactor, catalyst, methane, nanocarbon, modelling, optimization.

Ключевые слова: реактор, катализатор, метан, наноуглерод, моделирование, оптимизация.

 

INTRODUCTION

The influence of various factors on the synthesis of nanocarbon from the walnut peel, apricot kernel, methane, natural gas, and propane-butane fractions was studied, and the texture and sorption characteristics of the obtained nanocarbon were examined. The catalytic activity of the catalyst containing (CuO)x*(CoO)y*(NiO)z*(Fe2O3)k*(MoO3)m/HSZ prepared based on "zol-gel" technology for the implementation of processes was studied under differential reactor conditions. At the same time, the effect of various factors on the rate of formation of nanocarbon obtained from methane, natural gas, and propane-butane fractions was studied and optimal process conditions were proposed [1-6]. The physicochemical and operational properties of two industrial catalysts for nanocarbon synthesis were analyzed. Different methods: X-ray phase, chemical, and IR spectroscopy studied the composition of catalysts [7-10]. Chemical evaporation of carbon nanotubes (CVD) from a gas mixture consisting of methane (carbon precursor) and hydrogen (carrier gas) in the presence of catalytic particles on the scale of reactor length is modelled by solving surface chemistry problems. The model allows the determination of gas-phase areas, as well as surface coating and carbon deposition rates, by temperature, velocity, and different types. Various available experimental and theoretical evaluations are used to create the necessary database for gas-phase and surface chemistry and gas-phase transport parameters [11-29].

Thermocatalytic decomposition (TCD) of methane is being studied as a method of converting natural gas to hydrogen and functional carbon. In these processes, carbon is usually formed over the catalyst phase, leading to the growth of particles. Therefore, the development of a particle growth model is necessary to understand the thermocatalytic decomposition limitations of methane and to evaluate the optimal parameters and process conditions. A Multi-Grain Model (MGM) has been used to combine the effects of particle growth, kinetics, and internal heat and mass transfer [30 - 32]. Methane conversion in the reactor is calculated as a function of the longitudinal coordinate, temperature, and specific gas and catalyst flow rate of the specific carbon content and relative catalyst activity. At the specified specific methane flow rate, it is shown that there is an optimal specific catalyst flow with the maximum specific yield of carbon nanotubes, whereas in the combined reactor this efficiency is higher than in the countercurrent reactor [33-35]. A detailed microkinetic model and a digital methodology for combining Euler-Euler methods to simulate liquefied bed reactors have been proposed to the industry. Based on laboratory-scale experimental data, low losses (less than 10%) are achieved. In general, the work leads to the introduction of detailed kinetics in the simulation of industrial liquefied reactors [36, 37].

EXPERIMENTAL PART

The extraction of nano carbons from methane (Fe2(MoO4)3*MoO3) (cat №1) and (CuO)x*(CoO)y*(NiO)z*(Fe2O3)k*(MoO3)m/HSZ (cat №2) The catalyst containing (CuO)x*(CoO)y*(NiO)z*(Fe2O3)k*(MoO3)m/HSZ turned out to be more active compared to the previous layer №1, and experiments with it were carried out in a much lower temperature range. Cat №2 catalyst was prepared as follows:

 

Figure 1. Scheme of preparation of catalyst containing (CuO)x*(CoO)y*(NiO)z*(Fe2O3)k*(MoO3)m/HSZ

 

The essence of the method is the interaction of nitrate mixtures of metals included in the catalyst and the organic matter in the air at temperatures ≥500 ℃. The reaction is followed by the formation of finely dispersed oxides of metals.

The equations for changing the concentration of gas-phase components have the following form:

                                             (1)

where is –the linear velocity of the gas mixture, m/s;  - concentration of the i-component of the gas phase (i = 1 ... 3), mol/m3; - diffusion coefficient of the i-component of the gas phase, m2/s;  - the rate of formation or consumption of i-component according to the reactions that occur on the surface of the catalyst, mol/ (m3s); t - time, c; x - longitudinal coordinate of the reactor, m (counting head for the x axis - the point of entry of the gas phase into the apparatus).

The initial conditions of equation (1) are as follows:

                                                (2)

(2) states that the values of concentrations for each component of the gas phase at each point of the reactor at the initial moment are known.

The boundary conditions of equation (1) take into account the flow of reagents into the apparatus together with the initial gas mixture:

                                                    (3)

Where  - device length, m;  - initial gas component concentration at reactor inlet, mol/ m3. The equations for changing the concentration of the dispersed phase components are written as follows:

                                                      (4)

Where is  – the surface concentration of the solid phase component per unit mass of the catalyst, mol/kg; - the rate of formation or consumption of the i-component of the dispersed phase based on the reactions that occur on the catalyst’s surface, mol/ (kg ·s);  – the linear velocity of the dispersed phase, m/s (the minus sign indicates that the continuous and dispersed phases move in opposite current).

The initial conditions for solving equation (4) are written as follows:

                                                (5)

This is the distribution of the i-component concentration of the dispersed phase along the length of the apparatus at the initial moment of time, mol/kg.

In addition, to solve equation (4), it is necessary to have boundary conditions:

                                                   (6)

where is  – the surface concentration of the dispersed phase component at the reactor inlet, mol/kg.

Catalyst mass equilibrium equation:

                                               (7)

where is the mass of the catalyst, kg.

The initial conditions of equation (7) determine the mass distribution of the catalyst at time t = 0:

                                         (8)

The boundary conditions of equation (7) are written as follows:

                                               (9)

where - the mass of the catalyst at the entrance to the reactor, kg.

These mathematical models (1) -(9) allow one to calculate the concentration of system components not only at the outlet of the apparatus but also along the length of the reactor. Unlike a catalyst containing (Fe2(MoO4)3*MoO3), the dependence of the reaction rate on the gas velocity in the studied range of linear velocities of the initial gas mixture has only two areas: an increase in the rate of nano-fibre carbon formation was observed when the rate of methane delivery was increased at low linear velocities of the first field-initial gas mixture flow, and the rate of the reaction does not depend at velocities above 20 cm/min. The area of decrease

RESULTS AND THEIR DISCUSSION

We calculated the average reaction rate in the presence of this catalyst 25 min after the start of the experiment. The results of the experiment are shown in Figure 3. Unlike a catalyst containing (Fe2(MoO4)3*MoO3), the dependence of the reaction rate on the gas velocity in the studied range of linear velocities of the initial gas mixture has only two areas: an increase in the rate of nano-fibre carbon formation was observed when the rate of methane delivery was increased at low linear velocities of the first field-initial gas mixture flow, and the rate of the reaction does not depend at velocities above 20 cm/min. The area of decrease in the rate of formation of carbon layers in the catalyst has no experimental curves when the gas velocity is subsequently increased. This can be explained by the much higher activity of cat №2, which provides much higher rates of reactions in the catalyst. As a result, the methane supplied to the surface of the catalyst manages to interact with it before methane escapes with a stream of the initial gas mixture.

 

Figure 2. Cat №1 in the catalyst at various temperatures over time: 1 - 600 ℃; 2 – 650 ℃; 3 - 700 ℃ Variation in the specific gravity of methane from methane

 

In the above data, a graph of the change in the specific amount of carbon in the catalyst (Fe2(MoO4)3*MoO3) (cat №1) with increasing temperature over time is given. The figure shows the specific gravity of the carbon content in the catalyst at 600 oC, which is 22 g/g. But this takes longer (200 min). Again, this means that an increase in temperature leads to a decrease in catalyst activity (Figure 2).

 

 

Figure 3. At 25 minutes after the start of the experiment, the average rate of the nanocarbon synthesis reaction on the cat №2 catalyst was different at different temperatures: 1-600 ℃; 2-650 ℃ Dependence on the linear velocity of methane

 

As can be seen from Figure 3, the process must be carried out at linear velocities of not less than 25 cm/min of the initial gas mixture flow. Subsequent studies were performed on methane at a linear velocity of 35 cm/min.

The results of the study of the effect of temperature on the rate of nanocarbon synthesis showed that cat №2 differs from cat №1 in the catalyst. The application of cat №2 at lower temperatures allows nanocarbon to be obtained with a much higher specific yield, while the change in the specific amount of carbon in the catalyst is time-dependent and the kinetic curves have no induction period at all. The results of the experimental measurements are shown in Figure 4. The micro-images of the product obtained at a linear velocity of 35 cm/min of methane 2 hours after the start of the experiment at a temperature of 560 ℃ in a 10 mg solution of cat №2 catalyst are given in Figure 5. As can be seen, the product mainly represents nanocarbon with a diameter of 10 to 60 nm and a purity of about 98%. The image was obtained using an electron microscope, JEM-1400 (JEOL, Japan).

 

Figure 4. Cat №2 in the catalyst at various temperatures over time: 1 - 560 ℃; 2 – 580 ℃; 3 - 680 ℃ Change in the specific gravity of nanocarbon derived from methane

 

Figure 4 shows a graph of the change in temperature (CuO)x*(CoO)y*(NiO)z*(Fe2O3)k*(MoO3)m/HSZ (cat №2) at different temperatures over time as the catalyst increases. At 560 300 for 300 min, the catalyst exhibits its highest activity. At 560oC, the specific amount of carbon in the catalyst is 150 g/g. However, as the temperature rises (680 ℃), the specific gravity of the nanocarbon decreases sharply (68 g/g).

 

Figure 5. Micro-image of pyrolysis product of methane on cat №2 catalyst (temperature 560 ℃, catalyst mass 10 mg, methane linear velocity 35 cm/min)

 

Mathematical modelling of a methane catalytic pyrolysis continuous operating reactor. At present, there is almost no doubt that in the near future, the industry will need to produce high-yield and low-cost production of methane-derived nanocarbon. In this connection, the reaction of organizing the synthesis of methane-derived nanocarbon in a continuous mode seems very promising. This approach, in our opinion, improves the efficiency of these devices and, at the same time, reduces the cost of the finished product, methane-derived nanocarbon. To confirm these assumptions, it was decided to use a kinetic scheme of nanocarbon formation in the calculation of a continuously operating methane pyrolysis reactor (Table 1).

Table 1.

Kinetic constants of the model in cat №1 and cat №2 catalysts in mathematical modelling of the methane pyrolysis reactor

№ stages

cat №1

cat №2

kJ/mol

kJ/mol

103,5

56,6

2.

0,00107

10,3

425

10,0

3.

0,00107

10,3

425

10,0

4.

0,00107

10,3

425

10,0

5.

26100

6,62

5,1

6.

100,1

54,5

7.

124

72,6

6,15

64,1

8.

53,2

60,3

 

The continuous operation mode of the methane catalytic pyrolysis reactor is achieved by moving the catalyst layer along the device length with a countercurrent flow relative to the gas phase. In accordance with the kinetic scheme given in Table 1, we write the equations of change of concentrations for each of the components of the system:

 

 (4.18)

The equations of change of concentrations of gaseous components are written as follows:

Results of mathematical modelling of the reactor. The data presented in Table 1 and Figure 6 were used as the kinetic constants of the model in the mathematical modelling of a methane pyrolysis reactor with a moving catalyst.

 

Figure 6. Results of experimental studies of two catalysts in a continuous reactor (reactor temperature, 600 ℃)

 

The diameter of the reactor is 54 mm and the length of the heated part is 300 mm. The process temperature remained constant at 650 °C. The linear velocity of the gas supply (or its flow rate), as well as the catalyst flow rate, were varied.

 

Figure 7. Comparison of the results of mathematical modelling of a continuous reactor with experimental data (process temperature of 650 ℃)

 

Thus, real experiments were repeated using computer technology. The results of the calculations were compared with the experimental data, and the mathematical model developed demonstrated a good correlation between the experimental and calculated data in a continuous reactor using the kinetic constants selected for the reactor (Figure 6).

As shown in Figure 7, the best result in the presence of cat №1 is 5.1 g/h (in experiment 2), for cat №2 - 8.3 g/h (experiment 9). In this case, the yield of nanocarbon is 3.3 g/g and 13.4 g/g, respectively.

Figure 8 shows the change in the concentration of active centres along the length of the apparatus for each of the catalysts in experiments 2 and 9 (Table 2) at the steady-state of the process.

 

Figure 8. Active centres on the catalyst surface along the length of the reactor change in concentration, mol/kg: a -cat №1 (Experiment 2); b -floor №2 (Experiment 9).

 

The curve shown in Figure 8a is an almost straight line. This suggests that cat №1 active sites are consumed continuously throughout the entire process. The slope of this line characterizes the rate of consumption of the active centres of the catalyst and indicates that this figure is low. The change in the concentration of active centres on the surface of the cat №2 (Fig. 8b) has a clear curvilinear character. At the beginning of the process, the rate of consumption of the active centres of this catalyst is high and significantly exceeds the rate of consumption of the active centres of cat №2. As the catalyst passes from the reactor to the exit point, the rate of consumption of the active centres of cat №2 decreases, and the rate of cat ida1 at the output of the apparatus is close. In general, the cat №2 catalyst is used more efficiently in the methane pyrolysis process.

 

Figure 9. Variation of carbon concentration in the form of nanotubes on the surface of the catalyst along the length of the reactor, mol/kg: a - cat №1 (Experiment 2); b - floor №2 (Experiment 9).

 

Figure 9 shows the concentration of nanotubes along the length of the reactor for experiments 2 and 9. As can be seen from Figure 9a, the curve has an S-shaped appearance due to the presence of an induction circuit. This is also consistent with the results of the kinetic studies of the catalyst kat1, in which the kinetic curves recorded in the solid catalyst layer also include the induction period. The process of nanotube formation in the cat №2 catalyst (Fig. 9b) proceeds at a speed close to the maximum almost immediately after the catalyst enters the reactor, which once again demonstrates the efficiency of this catalyst.

Optimization of methane catalytic pyrolysis reactor. In determining the optimal conditions for the synthesis of methane in the catalytic pyrolysis reactor, it is important to determine the acceptance criteria and control parameters. The peculiarity of the nanocarbon production process is that the catalyst is consumed during the process. That is, the catalyst consumption is high with the low productivity of the nanocarbon, which does not allow the product to achieve a low cost. Therefore, it is important to take into account both nanocarbon output and reactor performance when selecting synthesis conditions. Process temperature and catalyst flow rate were taken as control parameters. In the calculations, the linear velocity of the gas phase was assumed to be 35 cm/min.

 

Figure 10. The specific yield of the product at a temperature of 650 °C and the dependence of the efficiency of the device on the consumption of the catalyst cat №1

 

As mentioned above, a series of experiments were performed to find the optimal values of process temperature and catalyst consumption. As a result, it was proved that the dependence of the final product efficiency and productivity on the consumption of the catalyst is of a different nature.

 

Figure 11. Cat №1 72 g/h the specific yield of the product at the catalyst consumption and the dependence of the device productivity on the process temperature

 

The temperature dependence of yield and productivity at constant catalyst consumption is the same - extreme nature (Fig.11).

Thus, it is not difficult to determine the optimum temperature of the process with the constant flow rate of the catalyst, because the maximum operation of the reactor and the output of the nanocarbon are achieved at the same temperature. Maximum yield and efficiency are achieved at different values of the process temperature when the consumption of the catalyst changes (Figure 9).

Table 2.

Different modes of nanocarbon synthesis from methane

Temperature ℃

Catalyst consumption, g/h

The yield of nanocarbon, g/g (%)

Nanocarbon consumption in the reactor, g/h (%)

cat №1

1

550

0.02

18,1 (100%)

0,36 (4,2%)

2

735

0.4

6,1 (33,7%)

8,6 (100%)

3

580

0,07

11 (60,5%)

5,2 (60,5%)

cat №2

1

550

0,05

69 (100%)

3,45(20,5%)

2

710

0,8

9,33(13,5%)

16,8(100%)

3

630

0,24

32 (46,5%)

7,8 (46,5%)

 

CONCLUSION

1. The effect of various factors (catalyst layer thickness, gas-phase linear velocity, and process temperature) on the product yield of the methane nanocarbon reaction from methane was studied.

2. Experimental values of specific gravity and efficiency of a reactor with continuous nanocarbon synthesis in cat №1 and cat №2 catalysts were obtained.

3. A mathematical model of nanocarbon formation during the catalytic pyrolysis of methane in a reactor with a mobile catalyst layer has been developed. This model allows one to determine the composition of nanocarbon and other surface compounds on the surface of the catalyst, the composition of the gas phase at any point in the apparatus, and the flow rate of each stage of the process.

4. From the kinetic scheme of Table 1, the developed mathematical model of a moving catalyst bed reactor was calculated using the kinetic constants selected for the two different catalysts and showed the compatibility of the experimental data.

5. The optimization results show the advantage of cat №2 catalyst over cat №1 in ensuring high values of nanofiber carbon yield and reactor performance.

 

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Информация об авторах

Doctoral student, Department of Physical and Colloid Chemistry, Samarkand State University, Republic Uzbekistan, Samarkand

докторант, кафедры физической и коллоидной химии, Самаркандского государственного университет, Республика Узбекистан, г. Самарканд

DSc, Professor, Department of Polymer Chemistry and Chemical Technology, Samarkand State University named after Sharof Rashidov, Republic Uzbekistan, Samarkand

д.т.н., профессор, кафедра химии полимеров и химической технологии, Самаркандский государственный университет имени Шарофа Рашидова, Республика Узбекистан, г. Самарканд

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