Journal of Multidisciplinary Engineering Science and Technology (JMEST)

ISSN: 2458-9403
Vol. 3 Issue 8, August - 2016

Modeling of steam methane reforming (SMR)

over a Ni-AL2O3 catalyst

Sajjad porgar Mohammad Tohidi pour

Dep: Chemical Engineering Dep: Chemical Engineering
Islamic Azad University South Tehran Branch Islamic Azad University South Tehran Branch
TEHRAN, IRAN TEHRAN, IRAN
St_s_porgar@azad.ac.ir m.tohidipour@gmail.com

Abstract—In present paper modeling of natural gas After desulfurization, natural gas and carbon dioxide
reforming by steam over nickel-alumina catalyst is mixed with water and flue gases and pre-heated to the
investigated and key parameters such as pressure, reaction temperature. Inside the reactor, there are long
temperature and mole ratio have been studied. The length and small diameter pipes with nickel-alumina
results show that the reforming performance is catalyst contained. Reforming conditions with a high
affected by temperature, pressure and ratio of temperature furnace are converted all hydrocarbons
steam to methane. The equations for mass and into products. In this process, the required carbon
energy balance equations and catalyst are dioxide usually achieved from returns all the carbon
mentioned. dioxide and also a significant amount of outside unit [2].
The combination of carbon monoxide and Process schematic is as follows:
hydrogen are known as syngas and are used as a
feedstock in the production of various products
such as ammonia and liquid fuel applications.
There are different techniques for the production of
synthesis gas. One of these techniques is dry
reforming that combination carbon dioxide and
methane are converted into synthesis gas.

Keywords—Natural gas, Reforming, Catalyst,

Steam
I.Introduction

The synthesis gas is odorless and colorless Figure 1- Process schematic [3]
poisonous gas that is a mixture of hydrogen and
carbon monoxide and use in various industries Steam reforming technology was used from 1920
including petrochemical and metallurgy industries. onwards, but from the 1950s onwards was used as a
There are several methods for the production of process for synthesis gas production of gas
synthesis gas from steam reforming of natural gas is compounds. The key point of these reactions is
mostly done with hydrocarbons such as naphtha. endothermic that require high temperatures and
Natural gas that primarily containing methane, reacts decomposition reaction of H-C band is the first
with water within tubular reactors at high temperature controller. As shown in the following equations
and absorb large amounts of heat, in the presence of C2+reactions (reaction I) are irreversible, but the
nickel-alumina catalyst and reaction final result is the decomposition of methane (reaction II) equilibrium
creation of reaction products and the ratio of relationship formed by the reaction of methane is
hydrogen to carbon monoxide is as the most returned to the reaction [4].
important criteria for reactor design process[1].
Modeling gas production reactor unit in the I: CnH2n+2 + nH2O ↔ nCO + (2n+1) H2
petrochemical industry is great importance.
II: CH4 + H2O ↔ CO + 3H2
II. Process described
Δ HII = +206 kJ/mol

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ISSN: 2458-9403
Vol. 3 Issue 8, August - 2016

III: CO + H2O ↔ CO2 + H2 catalytic reformer. Increase or decrease catalyst

temperature hurts catalyst grains physical form and
Δ HIII = - 41 kJ/mol expansion and contraction due to temperature drop
and increase in the launching primer reformer,
To achieve an appropriate level of transformation and
shattered grains catalyst, although has not major
product in the output current, the reaction is one
impact on the chemical activity of the catalyst or heat
temperature of 900-500°C and at pressure 40-30 bar.
transfer mode but increased pressure tubes and is
In this situation, reactions are quick but due to the need
reason for the replacement of the catalyst[7].
for stability and high mechanical resistance of the
Catalyst grains with different designs for a wide range
catalyst, penetrating into the pores of the catalyst is
of hydrocarbons is used and a different type of catalyst
relatively low and a high percentage of responses in the
used in the reformer stumbling at 1100-900°C works
catalyst grains carried out. Because this reaction is
used. Conventional fixed bed reformer has
endothermic for access to the appropriate conversion,
disadvantages such as low heat transfer rate, falling
shall be sufficient energy to gas to react to the move
resistance in the pores of the catalyst and
towards equilibrium for this purpose, standard reactors
nonisothermal. High endothermic reforming process of
can be built for gas reformer with a high number of
methane, a high impact on the efficiency of heat
tubes that catalyst poured into the tubes and the tubes
entering the reformer and the reformer can therefore be
around the burner tube temperature is raised and to
crucial, So choice reformer can be essential, apart from
supply reaction energy, diameter tubes are small and
the development of heat transfer, and mass transfer
uniform reaction will be done relatively[5]. Whatever
rate, high uniformity catalyst bed, can be advantages
tube diameter is less, the number of tubes mounted
to using fluid bed [8].
higher and will increase the heat transfer surface and
although reactions are quick, but the percent
III. Reaction kinetics
conversion of gas at the outlet tubes will not reach final.
To achieve complete conversion of methane to
hydrogen need to be very long tubes at the end of tubes Many equations for methane reforming reaction are
to reach equilibrium. Order to pressure drop in the presented by various researchers. In Table 2, the
reformer tubes primary, design catalysts with different number of relationships listed [9].
shape and size with adequate resistance against
breakage for this reason, the catalyst grains with large IV. Equations and modeling
holes in its surface have built and used in ammonia
units. The loss of yield and catalyst lifetime happens for Reactions are as follows:
several reasons: collected active compounds nickel is CH4 + H2O ↔ CO + 3H2
an unavoidable process and whatever the temperature
of the recovered metal catalyst increase, nickel will 𝑘1 𝑃𝐶𝐻4 𝑃𝐻2𝑂 𝑃𝐶𝑂 𝑃𝐻0.5
2
𝑟1 = − ( − ) [1]
more active on its base and accumulate in various parts 𝑑𝑒𝑛2 𝑃𝐻2.5
2
𝐾 1
caused the loss of active surface area of the metal.
−28870
When the primer feed containing impurities reformer 𝑘1 = 9.490 ∗ 1016 exp ( ) [2]
𝑇
catalyst poisoning is a possibility. Blocking the metal −26830
active site by materials toxic will stop cracking 𝐾1 = 10266.76 𝑒𝑥𝑝 ( ) [3]
𝑇
hydrocarbons operation. Sulfur is often a poison the k1= kg.h/ Kmol. KPa0.5
catalyst, sodium but there is in hydrocarbons or steam
and can not be removed easily and reacts with nickel K1= Pa2
bands that will reducing the effectiveness catalyst[6].
Other factors the loss of activity of the catalyst are Second reaction:
carbon and coke production that soot formation
mechanism depends on the temperature and CO + H2O ↔ CO2 +H2
composition of the gas and vapor on the catalyst. When
2 0.5
the steam to carbon ratio decreases significantly 𝑘3 𝑃𝐶𝐻4 𝑃𝐻 2𝑂
𝑃𝐶𝑂2 𝑃𝐻 2
𝑟3 = − ( 3.5 − ) [4]
𝑑𝑒𝑛2 𝑃𝐻 𝐾3
hydrocarbon feedstock in the form of coke or soot 2

began to break down (pyrolysis) and the soot on the

−8074.3
catalytic reformer sitting and increases the pressure 𝑘2 = 4.390 ∗ 104 exp ( ) [5]
𝑇
drop and the loss of activity of the catalyst. In some
cases, can be separated soot from the catalyst by −4400
injecting steam and often leads to the replacement 𝐾2 = exp ( − 4.036) [6]
𝑇
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Vol. 3 Issue 8, August - 2016

k2= kg.h/ Kmol. K Pa-1 T = Tin @ l = 0 [23]

Third reaction: 𝑈
1 1
CH4 + 2H2O ↔ CO2 + 4H2 𝐾𝑔 𝐷𝑝 𝐺 3 𝐶𝑝 𝜇 3
= 0.4 [2.58 ( ) ( )
𝐷𝑝 𝜇 𝐾𝑔
𝑘3 𝑃𝐶𝐻4 𝑃𝐻22𝑂 𝑃𝐶𝑂2 𝑃𝐻0.5
2
𝑟3 = − ( − ) [7] 0.4
𝑑𝑒𝑛2 𝑃𝐻3.5 𝐾 3
𝐷𝑝 𝐺 0.8 𝐶𝑝 𝜇
2 + 0.094 ( ) ( ) ] [24]
𝜇 𝐾𝑔
−29336
𝑘3 = 2.290 ∗ 1016 exp ( ) [8]
𝑇 Arrhenius equation:
K3= K1 * K2 𝐸
𝑘𝑖 = 𝐴𝑖 𝑒 −𝑅𝑇 , i = 1, 2, 3,… [25]
k3= kg.h/ Kmol. K Pa0.5
Vant Hoff equation:
K3= Pa2
𝐸
𝑘𝑗 = 𝐴𝑗 𝑒 −𝑅𝑇 , j = H2, CO , CO2 ,CH4 [26]
𝑑𝑒𝑛 = 1 + 𝐾𝐶𝑂 𝑃𝐶𝑂 + 𝐾𝐻2 𝑃𝐻2 + 𝐾𝐶𝐻4 𝑃𝐶𝐻4
𝑃 VII. The pressure drop in the reactor
+ 𝐾𝐻2𝑂 𝐻2 𝑂⁄𝑃 [9]
𝐻2
Because the reaction in a catalytic bed, the gas
−6
4604.28
𝐾𝐶𝐻4 = 6.65 ∗ 10 exp ( ) [10] pressure in the bed are facing. Pressure drop into bed
𝑇 it has an impact on the performance and efficiency [10].
−10666.356
𝐾𝐻2𝑂 = 1.77 ∗ 103 exp ( ) [11] 𝛿𝑃𝑡 𝑒𝑔 𝑣𝑠2
𝑇 = −10−5 𝑓 [27]
𝛿𝑧 𝑑𝑃
8497.71
𝐾𝐶𝑂 = 8.23 ∗ 10−7 exp ( ) [12] f from the following equation is obtained and also in
𝑇
terms of atmospheric pressure:
9971.13
𝐾𝐻2 = 6.12 ∗ 10−11 exp ( ) [13] 1 − 𝜀𝐵 𝑏(1 − 𝜀𝐵 )
𝑇
𝑓= [𝑎+ ] [28]
𝜀𝐵 𝑅𝑒
V. Mass balance
𝑅𝑒
𝑑𝑋𝐶𝑂2 𝜋 𝑑𝑖2 𝜌𝑏 𝑟𝐶𝑂2 𝑎 = 1.75 , 𝑏 = 150 , < 500 [29]
= ( ) [14] 1 − 𝜀𝐵
𝑑𝑙 4 𝐹
𝑅𝑒
𝑋𝐶𝑂2 = 0 @ 𝑙 = 0 [15] 𝑎 = 1.24 , 𝑏 = 368 , 1000 < < 5000 [30]
1 − 𝜀𝐵

𝑑𝑋𝐶𝐻4 𝜋 𝑑𝑖2 𝜌𝑏 𝑟𝐶𝐻4 4 𝑅𝑒

= ( ) [16] 𝑎 = 1.75 , 𝑏 = 5, ≥ 5000 [31]
𝑑𝑙 4 𝐹 1 − 𝜀𝐵
2𝑅𝑒 6

𝑋𝐶𝐻4 = 0 @ 𝑙 = 0 [17] VIII. Effectiveness factor

𝑟𝐶𝐻4 = 𝑟1 + 𝑟3 [18] For industrial catalysts that are large in size due to the
limited penetration velocity equation must be corrected
𝑟𝐶𝑂2 = 𝑟2 + 𝑟3 [19] that actual velocity of the particles obtained by
multiplying the impact factor [11]. The impact factor is
𝑑𝑋𝐶𝑂 𝜋 𝑑𝑖2 𝜌𝑏 𝑟𝐶𝑂 ratio of velocity in catalyst to velocity on the outer
= ( ) [20]
𝑑𝑙 4 𝐹 surface of the catalyst.

𝑋𝐶𝑂 = 0 @ 𝑙 = 0 [21] Assumptions that used in the effectiveness factor are

as follows:
VI. Energy balance  Catalyst particles are assumed spherical
shape.
dT 1 4U(Tw,i − T)
= [ + ρb ∑(∆HR ∗ r)] [22]
dl G Cp di

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 Catalyst particle throughout have the same

temperature. Table 1. The specific heat coefficient
i A B*103 C*106 D*106
𝑣 𝑑𝑣 CH2 1.702 9.081 -2.164 -
∫0 𝑟𝑖 (𝑃𝑡 )𝑒𝑔 𝑣
ɳ𝑖 = [32] H2 3.24 0.422 - 0.083
𝑟𝑖 (𝑃𝑡 𝑠 )𝑒𝑔
CO 3.376 0.557 - -0.031
Using equations expression for the dependent
CO2 3.475 1.045 - -1.157
components profiles obtained [12]: N2 3.28 0.593 - 0.04
Ps,CO -PCO =(De,CO2/Ds,CO)(PCO2 -Ps,CO2) – (De,CH4 /De,CO) H2O 3.47 1.45 - 0.121
(Ps,CH4 -PCH4) [33]
𝑁

λ𝐵 = (1 + 0.01P) ∑ 𝑦𝑖 𝜆𝑖 [43]
Ps,H2O–PH2O=(De,CO2/De,H2O)(PCO2-Ps,CO2)–(De,CH4/
𝑖
De,H2O) (Ps,CH4-PCH4) [34] 𝜆𝑖 = 𝐴 + 𝐵𝑇 + 𝐶𝑇 2 + 𝐷𝑇 3 [44]
λB = Thermal conductivity of an ideal gas mixture
Ps,H2 – PH2=(De,CO2/De,H2)(PCO2 – Ps,CO2) – (3De,CH4 /De,H2
XI. The viscosity of the ideal gas mixture
) (Ps,CH4 - PCH4) [35]

IX.Equations to calculate the physical properties The viscosity of the mixture can be obtained from the
of the fluid: following equation:
Assuming the gas will be ideal for mixed density: 𝜇𝐵 = ∑𝑁 1 𝑦𝑖 𝜇𝑖 [45]
𝑃𝑉 = 𝑛𝑅𝑇 [36] Viscosity is a function of temperature and pressure, but
𝑚 its dependence to the temperature is much more than
𝑛= [37] pressure and only in very high pressures change
𝑀
noticeable [13].
𝑅
𝑃 = 𝑐𝑅 𝑇 [38] From the following equation can be found on the
𝑀
temperature dependence of viscosity:
𝑁

𝑀 = ∑ 𝑦𝑖 𝑀𝑖 [39]
𝜇𝑖 × 𝐴𝐽 = [0.807 𝑇𝑟𝑖0.618 − 0.357 exp(−0.449𝑇𝑟𝑖 ) +
𝑖=1
0.34 exp(−4.035𝑇𝑟𝑖 ) + 0.18]𝐹𝑄∗ 𝐹𝑃∗ [46]
For an ideal gas specific heat the mixture is calculated 0.166
𝑇𝑐𝑖
as follows: 𝐴𝐽 = 0.176 { } [47]
𝑛
𝑀𝑖3 𝑃𝑐𝑖4
𝑖𝑔 𝑖𝑔
𝐶𝑝𝑅 = ∑ 𝑦𝑖 𝐶𝑝𝑖 [40] 𝐹𝑃∗ = 1 0 < 𝑑𝑟 < 0.022 [48]
𝑖=1
𝑖𝑔
𝑑𝑖2 𝑃𝑐𝑖
𝐶 𝑑𝑟𝑖 = 52.46 [49]
𝑝‫ه‬
= 𝐴 + 𝐵𝑇 + 𝐶𝑇 2 + 𝐷𝑇 −2 [41] 𝑇𝑐𝑖2
𝑅𝑇

yi= mole fraction of component i

D is momentum bipolar and 𝐹𝑄∗ for quantum gases are
X. The thermal conductivity of the mixture
defined as follows[14]:
𝐹𝑄∗ = 1.22 𝑄0.22 [ 1 + 0.00385 (𝑇𝑟 − 12)2 ] [50]
𝑁
Q(He) =1.38, Q(H2) = 0.76, Q( D2) = 0.52
𝜆𝐵 = ∑ 𝑦𝑖 𝜆𝑖 [42]
1
XII. Effective diffusion coefficient of components
λB = Thermal conductivity of an ideal gas mixture From the following equation can be obtaining effective
λi =Thermal conductivity of component i penetration into the catalyst grain [15]:
λi is a function of temperature and pressure and for one 𝜀𝑖
𝐷𝜀,𝑖 = 𝐷 [51]
bar the pressure will rise about 1%. 𝜏 𝑖
In relation τ is tortuosity and curvature of the catalyst
and ɛ is catalyst grains porosity. Di is calculated in
accordance with the following equation:
1 1 1
= + [52]
𝐷𝑖 𝐷𝑖𝑚 𝐷𝑖𝑘

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Table 4. Specification the reactor and catalyst

Penetration term of the Knudsen diffusion is calculated 0.1014 The inner diameter of the tube (m)
by the relationship 0.1320 The outer diameter of the tube (m)
𝜀𝑠 2 8𝑅𝑇 0.5 2.12 The total length of the tube (m)
𝐷𝑖𝑘 = 𝑎𝑝 [ ] [53]
𝜏 3 𝜋 𝑀𝑖 0.0172 Catalyst ring outer diameter (m)
0.01 Catalyst height (m)
Molecular effusion terms: 2.2355 Catalyst density (Kg/m 3)
𝑁
1 1 𝑦𝑗 0.528 ɛs
= ∑ [54] 3.54 Ʈ
𝐷𝑖𝑚 1 − 𝑦𝑖 𝐷𝑖𝑗
𝑗=2

Percent of methane and carbon dioxide by increasing

Two-component diffusion coefficient obtained from the
the inlet gas temperature decreases instead Percent of
following equation:
hydrogen and water vapor increases and this increase
1 1 1 1 in temperature reduces the pressure. If we reduce the
10−4 (1.084 − 0.249√𝑀 + 𝑀 ) 𝑇1.5 √𝑀 + 𝑀 )
𝑖 𝑗 𝑖 𝑗 pressure at constant temperature the same result will
𝐷𝑖𝑗 = [55]
𝑘𝑇 happen. Also by increasing the temperature in reactor
𝑃𝑡 𝑟𝑖𝑗 𝑓 ( )
𝜀𝑖𝑗′ input ratios H2O/CH4 and CO2/CH4 will remain
𝑟𝑖 +𝑟𝑗 constant, but the H2/CO ratio decreases. with
𝑟𝑖𝑗 = [56]
2
increasing temperature reaction goes to the water gas
𝜀𝑖𝑗′ = √𝜀𝑖′ 𝜀𝑗′ [57] shift reaction and produces H2 and CO with a ratio of
3and this ratio in reactor output decreases by
Table 2- Kinetic relationships offered by different
researchers: temperature increasing and eventually turns about one.
A ker and Camo −𝐸 Increasing the pressure at constant temperature or
(1995) −𝑟𝐶𝐻4 = 𝑘0 𝑒 𝑅𝑇 𝑃𝐶𝐻4 reducing the inlet gas temperature at a constant
Boudart (1967) −𝐸 pressure to increase percent of methane, and
−𝑟𝐶𝐻4 = 𝑘0 𝑒 𝑅𝑇 𝑃𝐶𝐻4
hydrogen and carbon monoxide and water vapor will
−𝐸
Allen (1975) −𝑟𝐶𝐻4 = 𝑘0 𝑒 𝑅𝑇 𝑃𝐶𝐻4 decrease. In water gas shift reaction does not change
−𝐸 the number of moles then pressure in this reaction is
−𝑟𝐶𝐻4 = 𝑘0 𝑒 𝑅𝑇 [𝑃𝐶𝐻4 not impressive but in reforming reaction is
Rostrup-Nielsen 𝑄𝑟
(1973) − (1 − ( ))] impressionable and is reducing H2/CO ratio.
𝐾𝑃 Due to the progress of the reaction in the presence of
excess water vapor, with increasing the amount of H2O
in the input, H2/CO ratio increases and decreases the
Table 3. Thermal Coefficient mole percent methane output.
i A B C D Operating pressure, temperature and molar ratio
H2 8.099*10-3 6.689*10-4 -4.158*10-7 1.562*10-20
H2O/CH4 and CO2/CH4 are influencing parameters at
CO 5.067*10-4 9.125*10-5 -3.524*10-8 8.199*10-12
the composition of the synthesis gas and for various
CO2 -7.21*10-3 8.015*10-5 5.477*10-9 -1.053*10-11 uses can be obtained by changing these parameters
H2O 7.64*10-3 -1.015*10-5 1.801*10-7 -9.1*10-11 different values. Basically, the reforming reaction is an
-4 -5 -8
N2 3.919*10 8.727*10 -5.067*10 1.504*10-11 endothermic reaction and therefore high temperature
CH4 -1.869*10-3 8.099*10-3 1.179*10-7 -3.614*10-11 will improve and further conversion of methane but role
of pressure is lower than other variables and therefore
it can be considered as a fixed parameter.
XIII. The Role of operating conditions
Table 5: constant values
In reforming reaction, the reaction in this entry indicates
that hydrocracking reactions occur according to the
A ( k1) A ( k2) A ( k3) A ( KCO) A ( K H2) A ( KCH2) A ( K H2O)
following reaction:
𝐶𝑘 𝐻2𝑘+2 + (𝑘 − 1)𝐻2 ↔ 𝑘𝐶𝐻4
Compounds heavier than methane are broken at the 4.225×1015 1.95×106 1.021×1015 8.2×10-5 6.2×10-9 6.6×10-2 1.8×105

entrance of the tube and produce methane. Because water gas shift reaction is exothermic
thereupon in a high-temperature reaction suppresses
so increase in temperature causes more methane into
H2 and CO, CO2 and convert CO into CO2 is less.

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Reforming reactions are equilibrium reactions therefore 8,1

composition of the feed heavily affects on the ratio of
8
CO/H2 production. Increasing the amount of CO2 in the

PH2( bar)
7,9
feed advances gas-water shift reaction and reduces in
7,8
CO/H2 production. By increasing the ratio of H2O/CH4 in
input, the ratio of CO2/CH4 constant in input and 7,7
temperature is constant and increases the ratio of CO/H2 7,6
production. By increasing of CO2/CH4 input in H2O/CH4 7,5
constant input and constant-temperature the CO/H2 7,4
ratio will reduce. 0 10 20 30
(E=6m) Length of catalyst
Table 6 -values of E and H vant Hoff and Arrhenius Figure 3 – H2 pressure on the length of the catalyst for
equation( kJ / mol) the (E= 6m)
E1 E2 E3 ∆HCO ∆HH2 ∆HCH4 ∆HH2O
241 66 23 -70 -81 -38 89 Becomes smaller catalyst particles in the pipes are
XIV. Conclusions reduced catalyst loading and increases the pressure
In the process, concentration gradient of gas drop across the bed.
component is limited to a very thin layer of the active In industry has always faced pressure restriction so can
catalyst. Catalyst component concentration gradient is built a catalyst with complex shapes in order to create
very steep in grain and mass transfer resistance more internal level, low pressure drop, or active
components in the catalyst grain are process controller. substances in the outer layer of the catalyst, on the one
hand improve the impact and also saving the use of
active metal that is usually expensive.
2
PCO2( bar)

1,75

1,5
0 10 20 30
(E=6m) Length of catalyst
Figure 1 - CO pressure on the length of the catalyst for the
Figure 4 – CO2 pressure on the length of the catalyst
(E=6m)
for the (E=6m)
Figure 2.Experimental data and model prediction
against the input oxygen flow for changes of methane 3
Ration of water to methane

conversion depicts. Irreversible reaction of methane to 2,5

produce CO or CO2 and water can increase the 2
conversion of methane to increase oxygen flow. 1,5
1
3,5 0,5
0
0,92 0,96 1 1,04 1,08 1,12
PCH4( bar)

The ratio of hydrogen to carbon monoxide

3 in output
Figure 5 - the ratio of in output to ratio of water to
methane

2,5 The ratio of hydrogen to carbon monoxide in reactor

0 5 10 15 design as a key parameter considered so for any
E=6m) Length of catalyst
change in this ratio changes to the percentage of feed
Figure 2 – CH4 pressure on the length of the catalyst for the
to be closer to the real standard.
(E=6m)

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80 0,015

methan concentration
The conversion of methane

70
0,01
60
50
0,005
40
30
0
0 5 10 15 20 25
2 4 06
input flow oxygen length of reactor
Figure10. Methane concentration changes in the
Figure 6 - Oxygen flow at input to the conversion of reactor length
methane
0,001

CO2 concentration
3 0,0008
Ratio of carbon dioxide to methane

2,5 0,0006
2 0,0004
1,5 0,0002

1 0
0 2 4
0,5 length of reactor
0 0,5 1 1,5 2
The ratio of hydrogen to carbon monoxide in output
Figure9. CO2 concentration changes in the reactor
Figure 7 - The ratio of in output of carbon dioxide length
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