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Prediction of non-isothermal ternary gas-phase breakthrough experiments based on binary data

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Abstract

The results of breakthrough experiments in an adsorption column packed with commercial activated carbon for three binary CO2/N2 mixtures as well as for two ternary CO2/N2/H2 mixtures are presented. The experiments were carried out at two different temperatures (25 and 45 °C), four different pressures (1, 5, 10 and 20 bar) and three different flow rates. To analyze the experiments, the breakthrough profiles are simulated using a one-dimensional model consisting of material and energy balances together with the necessary constitutive equations. Transport parameters such as the heat and mass transfer coefficients are fitted to the results from the experiments with the binary mixtures (CO2/N2) and then compared to parameters obtained in a previous work (Adsorption 18: 143–161, 2012) for binary CO2/H2 mixtures. Furthermore, the parameters obtained for binary mixtures are used to predict the outcome of breakthrough experiments with ternary CO2/N2/H2 mixtures. These simulations are then tested by experiments, showing that their prediction capability is rather satisfactory for a large range of experimental conditions.

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Abbreviations

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/(m3 K)]

C s :

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

C w :

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

D L :

Axial dispersion coefficient (m2/s)

d i :

Inner column diameter (m)

d o :

Outer column diameter (m)

d p :

Particle diameter (m)

\(\Updelta H\) :

Heat of adsorption (J/mol)

h L :

Heat transfer coefficient (lumping fluid phase + wall) [W/(m2 K)]

h w :

Heat transfer coefficient (lumping wall + heating) [W/(m2 K)]

k i :

Overall mass transfer coefficient (1/s)

K L :

Axial thermal conductivity in the fluid phase [W/(m K)]

L :

Column length (m)

N :

Number of species (–)

N meas :

Number of measured outputs (–)

N obs :

Number of measured observations (–)

N p :

Number of fitted parameters (–)

Nu:

Nusselt number

p :

Vector of parameters to be estimated

p* :

Optimal value of the fitted parameters

Δp* :

Fitting uncertainty of parameters p

p :

Fluid pressure (Pa)

q :

Solid phase concentration (mol/kg)

q eq :

Solid phase concentration at equilibrium (mol/kg)

R :

Ideal gas constant [J/(K mol)]

Re:

Reynolds number

t :

Time (s)

T :

Temperature (K)

T w :

Wall temperature, (K)

T amb :

Ambient temperature (K)

u :

Superficial gas velocity (m/s)

u set :

Superficial gas velocity setpoint given to the MFC (m/s)

y :

Mole fraction (–)

z :

Space coordinate in axial direction (m)

εb :

Bed void fraction (–)

εt :

Overall void fraction (–)

ɛMFC :

Uncertainty on the measured u set (m/s)

ɛset :

Deviation between fitted velocity and MFC setpoint (m/s)

η1, η2 :

Parameters for Leva’s correlation (–)

\(\Upphi\) :

Objective function (–)

μ:

Dynamic viscosity (Pa s)

ρ:

Fluid phase density (kg/m3)

ρ b :

Bulk density of the packing (kg/m3)

ρ p :

Particle density (kg/m3)

i :

Component i

F :

Feed

0:

Initial

BPR:

Back pressure regulator

CCS:

Carbon capture and storage

EOS:

Equation of state

IGCC:

Integrated gasification combined cycle

MFC:

Mass flow controller

MLE:

Maximum likelihood estimate

MS:

Mass spectrometer

PSA:

Pressure swing adsorption

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Acknowledgments

Partial support of the Swiss National Science Foundation through grant NF 200021-130186 and of the Commission for Technology and Innovation through grant CTI no. 12903.1 is gratefully acknowledged.

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Authors and Affiliations

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

    Dorian Marx, Lisa Joss, Nathalie Casas, Johanna Schell & Marco Mazzotti

Authors
  1. Dorian Marx
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  2. Lisa Joss
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  3. Nathalie Casas
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  4. Johanna Schell
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  5. Marco Mazzotti
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Correspondence to Dorian Marx.

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Marx, D., Joss, L., Casas, N. et al. Prediction of non-isothermal ternary gas-phase breakthrough experiments based on binary data. Adsorption 20, 493–510 (2014). https://doi.org/10.1007/s10450-013-9593-5

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  • DOI: https://doi.org/10.1007/s10450-013-9593-5

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