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Study of effectiveness factors with non-uniform catalyst distributions for methane steam reforming

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Abstract

In the present work, three kinetic expressions for methane steam reforming with different methane and water partial pressures dependence were studied. Methane effectiveness factors were simulated for spherical uniform pellets (those customarily employed), for several temperatures and water/methane ratios (hereafter called R). It was found that all effectiveness factors decreased with temperature as expected for all the kinetics expressions studied. On the other hand, the evolution with R was strongly dependent on the kinetics analyzed, with an important change in effectiveness factors values, ranging from 30 to 400%. This implies that the most convenient active sites distribution might be dependent on R evolution throughout the reactor. Then, two MSR reactors were simulated, loaded with pelletized catalysts with uniform and eggshell in order to get uniform nomenclature active site distributions. It was found that the one loaded with eggshell in order to get uniform nomenclature pellets saves up to 30% catalysts mass with respect to the uniform catalyst distribution for the same CH4 conversion, reinforcing the importance of active sites distribution.

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Abbreviations

DFT:

Density functional theory

DRM:

Dry reforming of methane

MSR:

Methane steam reforming

C [mol m3]:

Molar concentration

Cp [J mol−1 K−1]:

Molar heat capacity

D [m2 s−1]:

Diffusivity

DK [m2 s−1]:

Knudsen diffusivity

F [mol s−1]:

Molar flow

H [-]:

Heaviside step function

ΔH [J mol−1]:

Heat of reaction

k []:

Specific reaction constant

K []:

Equilibrium constant

L [m]:

Pellet size

M [kg]:

Catalyst mass

N [mol s−1 m−2]:

Molar flux

P [atm]:

Pressure

q [W s−1 m−2]:

Heat flux

r [mol s−1 m−3]:

Reaction rate

R [-]:

Water to methane feed ratio

Rc [atm L mol−1 K−1]:

Universal gas constant

T [K]:

Temperature

z [m]:

Spatial coordinate

α [-]:

Stoichiometric factor

κ [W m−1 K−1]:

Thermal conductivity

η [-]:

Effectiveness factor

*:

Indicates dimensionless variable

a:

Active phase left boundary

b:

Active phase right boundary

i:

Reaction

j:

Species

s:

At the surface conditions

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Funding

Authors thank to Universidad of Buenos Aires and Consejo Nacional de Investigaciones Científicas y Técnicas CONICET for their financial support.

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  1. Instituto de Tecnologías del Hidrógeno y Energías Sostenibles, ITHES (UBA-CONICET), Pabellón de Industrias, Ciudad Universitaria, 1428, Ciudad Autónoma de Buenos Aires, Argentina

    Ignacio Iglesias, Eduardo Poggio-Fraccari & Pablo Giunta

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  1. Ignacio Iglesias
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  2. Eduardo Poggio-Fraccari
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  3. Pablo Giunta
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Correspondence to Eduardo Poggio-Fraccari.

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Iglesias, I., Poggio-Fraccari, E. & Giunta, P. Study of effectiveness factors with non-uniform catalyst distributions for methane steam reforming. Reac Kinet Mech Cat 130, 713–726 (2020). https://doi.org/10.1007/s11144-020-01822-8

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