Abstract
The adsorption uptake curves of CO2, CO, N2 and CH4 on zeolite LiX and activated carbon were measured using a volumetric method at 293, 308 and 323 K and pressure up to 100 kPa. The experimental uptake curves were correlated with a non-isothermal kinetic model because the adsorption kinetics was controlled by heat generation and transfer, and an isothermal model showed large deviation from experimental uptake. The adsorption rates of the gases on zeolite LiX and activated carbon were affected by the isosteric heat of adsorption, heat transfer rate and adsorption affinity. At the same pressure and temperature, the sequence of effective diffusion time constants was CO2 ≪ CO < N2 < CH4 for zeolite LiX and CO2 ≪ CH4 ≤ N2 < CO for activated carbon. The adsorption rate of CO showed the largest difference between the two adsorbents. Effective diffusion time constants (D/R2) for all cases were provided, which depended on pressure and temperature.
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Abbreviations
- a:
-
External surface area divided by the volume of the adsorbent (m−1)
- cp :
-
Concentration in the particle (mol kg−1)
- Cs :
-
Heat capacity of the sample (J g−1 K−1)
- D/R2 :
-
Effective diffusion time constant (s−1)
- D:
-
Diffusivity (m2 s−1)
- Dc/rc :
-
Micropore diffusion time constant (s−1)
- Dp/Rp :
-
Effective macropore diffusion time constant (s−1)
- h:
-
Overall heat transfer coefficient (J m−1 s−1 K−1)
- K:
-
Henry constant (–)
- P:
-
Pressure (kPa)
- Q:
-
Adsorbed amount (mol kg−1)
- Qst :
-
Isosteric heat of adsorption (kJ mol−1)
- R:
-
Ideal gas constant (J mol−1 K−1)
- R2 :
-
Coefficient of determination (R2) (–)
- T:
-
Time (s)
- T:
-
Temperature (K)
- Vg :
-
Volume occupied by the gas (m3)
- Vs :
-
Volume occupied by the adsorbent (m3)
- α:
-
Dimensionless parameter defined by non-isothermal model (–)
- β:
-
Dimensionless parameter defined by non-isothermal model (–)
- ρs :
-
Density of the adsorbent (g m−3)
- 0:
-
Initial state
- ∞:
-
Equilibrium state
References
Ahn, H., Moon, J.-H., Hyun, S.-H., Lee, C.-H.: Diffusion mechanism of carbon dioxide in zeolite 4A and CaX pellets. Adsorption 10(2), 111–128 (2004)
Ahn, H., Yang, J., Lee, C.-H.: Effects of feed composition of coke oven gas on a layered bed H2 PSA process. Adsorption 7(4), 339–356 (2001)
Ahn, H., Yoo, H.-K., Shul, Y., Hyun, S., Lee, C.-H.: Diffusion mechanism of N2 and CH4 in pelletized zeolite 4A, 5A and CaX. J. Chem. Eng. Jpn. 35(4), 334–345 (2002)
Ahn, S., You, Y.-W., Lee, D.-G., Kim, K.-H., Oh, M., Lee, C.-H.: Layered two-and four-bed PSA processes for H2 recovery from coal gas. Chem. Eng. Sci. 68(1), 413–423 (2012)
Bae, Y.-S., Lee, C.-H.: Sorption kinetics of eight gases on a carbon molecular sieve at elevated pressure. Carbon 43(1), 95–107 (2005)
Cavenati, S., Grande, C.A., Rodrigues, A.E.: Separation of CH4/CO2/N2 mixtures by layered pressure swing adsorption for upgrade of natural gas. Chem. Eng. Sci. 61(12), 3893–3906 (2006)
Crank, J.: The Mathematics of Diffusion. Oxford University Press, London (1956)
Do, D.D.: Adsorption Analysis: Equilibria and Kinetics, vol. 2. Imperial College Press, London (1998)
Giesy, T.J., LeVan, M.D.: Mass transfer rates of oxygen, nitrogen, and argon in carbon molecular sieves determined by pressure-swing frequency response. Chem. Eng. Sci. 90, 250–257 (2013)
Grande, C.A., Rodrigues, A.E.: Layered vacuum pressure-swing adsorption for biogas upgrading. Ind. Eng. Chem. Res. 46(23), 7844–7848 (2007)
Gray, P.G., Do, D.D.: Dynamics of carbon dioxide sorption on activated-carbon particles. AIChE J. 37(7), 1027–1034 (1991)
Himeno, S., Komatsu, T., Fujita, S.: High-pressure adsorption equilibria of methane and carbon dioxide on several activated carbons. J. Chem. Eng. Data 50(2), 369–376 (2005)
Hu, X., Mangano, E., Friedrich, D., Ahn, H., Brandani, S.: Diffusion mechanism of CO2 in 13X zeolite beads. Adsorption 20(1), 121–135 (2014)
Kočiřík, M., Struve, P., Bülow, M.: Analytical solution of simultaneous mass and heat transfer in zeolite crystals under constant-volume/variable-pressure conditions. J. Chem. Soc. Faraday Trans. 1 80(8), 2167–2174 (1984)
Lee, H.-H., Lee, J.-C., Joo, Y.-J., Oh, M., Lee, C.-H.: Dynamic modeling of Shell entrained flow gasifier in an integrated gasification combined cycle process. Appl. Energy 131, 425–440 (2014a)
Lee, J.C., Lee, H.H., Joo, Y.J., Lee, C.H., Oh, M.: Process simulation and thermodynamic analysis of an IGCC (integrated gasification combined cycle) plant with an entrained coal gasifier. Energy 64, 58–68 (2014b)
Lee, J.J., Kim, M.K., Lee, D.G., Ahn, H., Kim, M.J., Lee, C.H.: Heat-exchange pressure swing adsorption process for hydrogen separation. AIChE J. 54(8), 2054–2064 (2008)
Lee, L.-K., Ruthven, D.M.: Analysis of thermal effects in adsorption rate measurements. J. Chem. Soc. Faraday Trans. 1(75), 2406–2422 (1979)
Linstrom, P., Mallard, W.: NIST Chemistry Webbook. NIST Standard Reference Database No. 69 (2001)
Park, Y., Moon, D.-K., Kim, Y.-H., Ahn, H., Lee, C.-H.: Adsorption isotherms of CO2, CO, N2, CH4, Ar and H2 on activated carbon and zeolite LiX up to 1.0 MPa. Adsorption 20(4), 631–647 (2014)
Ruthven, D.M., Lee, L.K., Yucel, H.: Kinetics of non-isothermal sorption in molecular sieve crystals. AIChE J. 26(1), 16–23 (1980)
Silva, J.A., Schumann, K., Rodrigues, A.E.: Sorption and kinetics of CO2 and CH4 in binderless beads of 13X zeolite. Microporous Mesoporous Mater. 158, 219–228 (2012)
Siriwardane, R.V., Shen, M.-S., Fisher, E.P., Poston, J.A.: Adsorption of CO2 on molecular sieves and activated carbon. Energy Fuels 15(2), 279–284 (2001)
Yang, J., Lee, C.H.: Adsorption dynamics of a layered bed PSA for H2 recovery from coke oven gas. AIChE J. 44(6), 1325–1334 (1998)
Yang, Y., Ribeiro, A.M., Li, P., Yu, J.-G., Rodrigues, A.E.: Adsorption equilibrium and kinetics of methane and nitrogen on carbon molecular sieve. Ind. Eng. Chem. Res. 53(43), 16840–16850 (2014)
You, Y.-W., Lee, D.-G., Yoon, K.-Y., Moon, D.-K., Kim, S.M., Lee, C.-H.: H2 PSA purifier for CO removal from hydrogen mixtures. Int. J. Hydrogen Energy 37(23), 18175–18186 (2012)
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We would like to acknowledge the financial support from the R&D Convergence Program of MSIP (Ministry of Science, ICT and Future Planning) and NST (National Research Council of Science & Technology) of Republic of Korea (CRC-14-1-KRICT).
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Ju, Y., Park, Y., Park, D. et al. Adsorption kinetics of CO2, CO, N2 and CH4 on zeolite LiX pellet and activated carbon granule. Adsorption 21, 419–432 (2015). https://doi.org/10.1007/s10450-015-9683-7
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DOI: https://doi.org/10.1007/s10450-015-9683-7