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Fixed bed adsorption of CO2/H2 mixtures on activated carbon: experiments and modeling

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Abstract

We present breakthrough experiments in a fixed bed adsorber packed with commercial activated carbon involving feed mixtures of carbon dioxide and hydrogen of different compositions. The experiments are carried out at four different temperatures (25 °C, 45 °C, 65 °C and 100 °C) and seven different pressures (1 bar, 5 bar, 10 bar, 15 bar, 20 bar, 25 bar and 35 bar). The interpretation of the experimental data is done by describing the adsorption process with a detailed one-dimensional model consisting of mass and heat balances and several constitutive equations, such as an adsorption isotherm and an equation of state. The dynamic model parameters, i.e. mass and heat transfer, are fitted to one single experiment (reference experiment) and the model is then further validated by predicting the remaining experiments. Furthermore, the choice of the isotherm model is discussed. The assessment of the model accuracy is carried out by comparing simulation results and experimental data, and by discussing key features and critical aspects of the model. This study is valuable per se and a necessary step toward the design, development and optimization of a pressure swing adsorption process for the separation of CO2 and H2 for example in the context of a pre-combustion CO2 capture process, such as the integrated gasification combined cycle technology.

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Abbreviations

a p :

specific surface of the adsorbent particles, [m2/m3]

a w :

cross section of the column wall, [m2]

c :

fluid phase concentration, [mol/m3]

C ads :

heat capacity of the adsorbed phase, [J/(K kg)]

C g :

heat capacity of the gas, [J/(K m3)]

\(C_{\mathrm{g}}^{\mathrm{mol}}\) :

specific heat capacity of the gas, [J/(K mol)]

C s :

heat capacity of the solid, [J/(K kg)]

C w :

lumped heat capacity of the wall, [J/(K m3)]

D e :

effective diffusion coefficient into the adsorbent particles [m2/s]

D L :

axial dispersion coefficient [m2/s]

D m :

molecular diffusion coefficient [m2/s]

d p :

particle diameter, [m]

ΔH :

heat of adsorption, [J/mol]

h L :

heat transfer coefficient (lumping column inside + wall), [J/(m2 s K)]

h W :

heat transfer coefficient (lumping wall + heating), [J/(m2 s K)]

k :

overall mass transfer coefficient, [1/s]

K :

Langmuir equilibrium constant, [1/Pa]

K L :

effective axial thermal conductivity in the fluid phase, [J/(m s K)]

L :

column length [m]

N :

number of species, [–]

N vol :

number of volume elements in the column, [–]

p :

fluid pressure, [Pa]

q :

solid phase concentration, [mol/kg]

q ∗ :

solid phase concentration at equilibrium, [mol/kg]

q s :

solid phase concentration at saturation, [mol/kg]

R :

ideal gas constant, [J/(K mol)]

R i :

inner column radius, [m]

R o :

outer column radius, [m]

s :

exponent in Sips isotherm [–]

s 1 :

parameter for temperature dependent description of s, [–]

s 2 :

parameter for temperature dependent description of s, [–]

t :

time, [s]

T :

temperature, [K]

T w :

wall temperature, [K]

T amb :

ambient temperature, [K]

u :

superficial gas velocity, [m/s]

y :

mole fraction, [–]

z :

space coordinate in axial direction, [m]

ε b :

bed void fraction, [–]

ε t :

overall void fraction, [–]

θ :

parameter for temperature dependent description of q s, [J/mol]

Θ :

parameter for temperature dependent description of K, [J/mol]

μ :

dynamic viscosity, [Pas]

ρ :

fluid phase density, [kg/m3]

ρ b :

bulk density of the packing, [kg/m3]

ρ p :

particle density, [kg/m3]

ω :

parameter for temperature dependent description of q s, [mol/kg]

Ω :

parameter for temperature dependent description of K, [1/Pa]

feed:

feed

i :

component i

init:

initial

j :

component j

pipe:

piping

BPR:

back pressure regulator

CCS:

Carbon Capture and Storage

EOS:

Equation of State

IGCC:

Integrated Gasification Combined Cycle

MSB:

magnetic suspension balance

MFC:

mass flow controller

MS:

mass spectrometer

PDE:

Partial Differential Equations

PSA:

Pressure Swing Adsorption

TSA:

Temperature Swing Adsorption

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Acknowledgements

This research has received funding from the European Union’s Seventh Framework Program (FP7/2007-2011) under grant agreement n∘211971 (the DECARBit project)

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Authors and Affiliations

  1. Institute of Process Engineering, ETH Zurich, Sonneggstrasse 3, 8092, Zurich, Switzerland

    Nathalie Casas, Johanna Schell & Marco Mazzotti

  2. Department of Energy Resources Engineering, Stanford University, Stanford, USA

    Ronny Pini

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  1. Nathalie Casas
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  2. Johanna Schell
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  3. Ronny Pini
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  4. Marco Mazzotti
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Correspondence to Marco Mazzotti.

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Casas, N., Schell, J., Pini, R. et al. Fixed bed adsorption of CO2/H2 mixtures on activated carbon: experiments and modeling. Adsorption 18, 143–161 (2012). https://doi.org/10.1007/s10450-012-9389-z

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