TY - JOUR
T1 - Effective model for olefin/paraffin separation using (Co, Fe, Mn, Ni)-MOF-74
AU - Luna-Triguero, Azahara
AU - Vicent Luna, Jose Manuel
AU - Becker, Tim
AU - Vlugt, Thijs
AU - Dubbeldam, David
AU - Gomez-Alvarez, Paula
AU - Calero, Sofia
N1 - Accepted Author Manuscript
PY - 2017
Y1 - 2017
N2 - An increase in demand for energy efficient processes for the separation of saturated and unsaturated light hydrocarbons mixtures drives the need of noncryogenic processes. The adsorptive separation using Metal-Organic Frameworks with coordinatively unsaturated metal sites may provide a cost-effective alternative due to the strong binding of the metal cation with the unsaturated hydrocarbons. Since experiments on adsorption equilibrium of gas mixtures are challenging, we propose classical force field based simulations to analyse the ability of MOF-74 with different metal substitutions for the separation of C2 and C3 olefin/paraffin binary mixtures. We parametrized the force field by fitting to available experimental single-component adsorption isotherms of ethane, ethene, propane, and propene in M–MOF-74 (M=Co, Fe, Mn, and Ni). The force field was validated for a variety of temperatures ranged from 273 K to 353 K. We then conducted Monte Carlo simulations in the Grand-Canonical ensemble to elucidate the adsorption mechanisms of the saturated/unsaturated hydrocarbon mixtures, at 318 K and 353 K. We computed the adsorption isotherms, and from these the adsorption selectivity, and addressed the variations of MOF properties with different metal cations. Fe-based MOF-74 appears the best option for both ethane/ethene and propane/propene separation applications. This finding partly agrees with previous work based on the Ideal Adsorbed Solution Theory.
AB - An increase in demand for energy efficient processes for the separation of saturated and unsaturated light hydrocarbons mixtures drives the need of noncryogenic processes. The adsorptive separation using Metal-Organic Frameworks with coordinatively unsaturated metal sites may provide a cost-effective alternative due to the strong binding of the metal cation with the unsaturated hydrocarbons. Since experiments on adsorption equilibrium of gas mixtures are challenging, we propose classical force field based simulations to analyse the ability of MOF-74 with different metal substitutions for the separation of C2 and C3 olefin/paraffin binary mixtures. We parametrized the force field by fitting to available experimental single-component adsorption isotherms of ethane, ethene, propane, and propene in M–MOF-74 (M=Co, Fe, Mn, and Ni). The force field was validated for a variety of temperatures ranged from 273 K to 353 K. We then conducted Monte Carlo simulations in the Grand-Canonical ensemble to elucidate the adsorption mechanisms of the saturated/unsaturated hydrocarbon mixtures, at 318 K and 353 K. We computed the adsorption isotherms, and from these the adsorption selectivity, and addressed the variations of MOF properties with different metal cations. Fe-based MOF-74 appears the best option for both ethane/ethene and propane/propene separation applications. This finding partly agrees with previous work based on the Ideal Adsorbed Solution Theory.
KW - adsorption
KW - hydrocarbon separation
KW - molecular simulation
KW - open-metal site
UR - http://resolver.tudelft.nl/uuid:0cd6cd5e-b415-47a0-87a9-2be5445ac505
U2 - 10.1002/slct.201601095
DO - 10.1002/slct.201601095
M3 - Article
SN - 2365-6549
VL - 2
SP - 665
EP - 672
JO - ChemistrySelect
JF - ChemistrySelect
IS - 2
ER -