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Binary adsorption behaviour of methane and nitrogen gases

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Abstract

Separation of methane and nitrogen gases is critical in the upgrading of LFG (Landfill gas), natural gas and coal bed gas in order to have a commercial heating value for methane. From an environmental point of view, methane capture from landfill gas is essential to prevent greenhouse gas emissions. Adsorption could be a beneficial process to capture low purity methane from a landfill site that is nearing the end of its lifecycle and produce high purity methane. In this work, Ceca 13X zeolite and Alcan Activated Alumina AA 320-AP have been studied for their potential for this separation and compared with Silicalite in literature. Pure and mixture adsorption isotherms were determined at 40 and 100 °C for these adsorbents by constant volume method and concentration pulse chromatographic technique, respectively. Mixture adsorption isotherms for the binary system of methane and nitrogen gases at 40 and 100 °C and 1 atmosphere total pressure have been determined by VV–CPM (Van der Vlist and Van der Meijden Concentration Pulse Method). The application of Extended Langmuir model for this binary system have also been discussed and compared to the experimental results. Results show that equilibrium separation factor for silicalite is larger than zeolite Ceca 13X and Alcan activated alumina AA320-AP. Both Silicalite and Ceca 13X find application in the bulk separation of methane from nitrogen when y CH4 > 0.4, especially in LFG, coal bed gas and natural gas.

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Abbreviations

a i :

Coefficients for Eq. 6 (mmol/g/atm)

b i :

Coefficients for Eq. 7 (mmol/g/atm)

B :

Adsorption affinity constant (/atm)

B i :

Adsorption affinity constant for component ‘i’ (/atm)

c :

Sorbate concentration in bulk phase (mol/cm3)

G i :

Coefficients for Eq. 5 (mmol/g/atm)

K :

Dimensionless Henry’s law constant (dimensionless)

K p :

Dimensional Henry’s law constant (mmole/g/atm)

L :

Length of the chromatographic column (cm)

P :

(total) Pressure (atm)

P 1 :

Partial pressure of Component 1 (atm)

P 2 :

Partial pressure of Component 2 (atm)

q 0 i :

Amount adsorbed of pure gas component ‘i’ (mmol/g)

q :

Amount adsorbed (mmol/g)

q 1 :

Amount adsorbed of Component 1 (mmol/g)

q 2 :

Amount adsorbed of Component 2 (mmol/g)

q m :

Adsorption saturation capacity or maximum amount adsorbed (mmol/g)

q m1 :

Adsorption saturation capacity or maximum amount adsorbed for component 1 (mmol/g)

R :

Gas constant (8.314 J/K/mol)

t :

Time (s)

T :

Temperature (K)

x :

Mole fraction in adsorbed phase at equilibrium (dimensionless)

x 1 :

Mole fraction of component 1 in adsorbed phase at equilibrium = q 1/(q 1 + q 2) (dimensionless)

x 2 :

Mole fraction of Component 2 in adsorbed phase at equilibrium = q 2/(q 1 + q 2) (dimensionless)

y :

Mole fraction in fluid phase at equilibrium (dimensionless)

y 1 :

Mole fraction of Component 1 in fluid phase at equilibrium (dimensionless)

y 2 :

Mole fraction of Component 2 in fluid phase at equilibrium (dimensionless)

α1/2 :

Separation factor (the ratio of Component 1 over Component 2) (dimensionless)

ε:

Porosity of the bed (dimensionless)

θ :

Fraction of monolayer coverage (dimensionless)

μ:

First moment (Average retention time) (s)

μ D :

System dead time (s)

v :

Interstitial fluid velocity (cm/s)

ρ :

Density of adsorbent (without pores) (g/cc)

CH4 :

Methane

CPM:

Concentration pulse method

GC:

Gas chromatograph

He:

Helium

HT:

Harlick-Tezel

LFG:

Landfill gas

MFC:

Mass flow controller

N2 :

Nitrogen

NI:

National instruments

PSA:

Pressure swing adsorption

TCD:

Thermal conductivity detector

TSA:

Temperature swing adsorption

VV:

Van der Vlist and Van der Meijden

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Acknowledgments

Financial supports received from Ontario Centres of Excellence (OCE), RioTinto Alcan and Air Products & Chemicals Inc., are gratefully acknowledged.

Author information

Authors and Affiliations

  1. Department of Chemical and Biological Engineering, Doosan Power Systems, Porterfield Rd., Renfrew, PA4 8DJ, Scotland, UK

    V. P. Mulgundmath

  2. Department of Chemical and Biological Engineering, University of Ottawa, 161, Louis Pasteur, Ottawa, K1N 6N5, Canada

    F. H. Tezel

  3. SilverBirch Hotels and Resorts, 161, Louis Pasteur, Ottawa, K1N 6N5, Canada

    F. Hou

  4. Air Products and Chemicals, Inc., 7201, Hamilton Blvd., Allentown, PA, 18195-1501, USA

    T. C. Golden

Authors
  1. V. P. Mulgundmath
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  2. F. H. Tezel
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Correspondence to F. H. Tezel.

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Mulgundmath, V.P., Tezel, F.H., Hou, F. et al. Binary adsorption behaviour of methane and nitrogen gases. J Porous Mater 19, 455–464 (2012). https://doi.org/10.1007/s10934-011-9494-5

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