Biporous Metal-Organic Framework with Tunable CO 2 /CH 4 Separation Performance Facilitated by Intrinsic Flexibility.

Autor: Gładysiak A; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland., Deeg KS; Department of Chemistry , University of California , Berkeley , California 94720 , United States., Dovgaliuk I; Swiss-Norwegian Beamlines , European Synchrotron Radiation Facility , 38000 Grenoble , France., Chidambaram A; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland., Ordiz K; Department of Chemical and Biomolecular Engineering , University of California , Berkeley , California 94720 , United States., Boyd PG; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland., Moosavi SM; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland., Ongari D; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland., Navarro JAR; Departamento de Química Inorgánica , Universidad de Granada , Av. Fuentenueva S/N , 18071 Granada , Spain., Smit B; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland.; Department of Chemistry , University of California , Berkeley , California 94720 , United States.; Department of Chemical and Biomolecular Engineering , University of California , Berkeley , California 94720 , United States., Stylianou KC; Laboratory of Molecular Simulation (LSMO), Institut des sciences et ingénierie chimiques (ISIC) , École polytechnique fédérale de Lausanne (EPFL) Valais , Rue de l'Industrie 17 , 1951 Sion , Switzerland.
Jazyk: angličtina
Zdroj: ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2018 Oct 24; Vol. 10 (42), pp. 36144-36156. Date of Electronic Publication: 2018 Oct 11.
DOI: 10.1021/acsami.8b13362
Abstrakt: In this work, we report the synthesis of SION-8, a novel metal-organic framework (MOF) based on Ca(II) and a tetracarboxylate ligand TBAPy 4- endowed with two chemically distinct types of pores characterized by their hydrophobic and hydrophilic properties. By altering the activation conditions, we gained access to two bulk materials: the fully activated SION-8F and the partially activated SION-8P with exclusively the hydrophobic pores activated. SION-8P shows high affinity for both CO 2 ( Q st = 28.4 kJ/mol) and CH 4 ( Q st = 21.4 kJ/mol), while upon full activation, the difference in affinity for CO 2 ( Q st = 23.4 kJ/mol) and CH 4 ( Q st = 16.0 kJ/mol) is more pronounced. The intrinsic flexibility of both materials results in complex adsorption behavior and greater adsorption of gas molecules than if the materials were rigid. Their CO 2 /CH 4 separation performance was tested in fixed-bed breakthrough experiments using binary gas mixtures of different compositions and rationalized in terms of molecular interactions. SION-8F showed a 40-160% increase (depending on the temperature and the gas mixture composition probed) of the CO 2 /CH 4 dynamic breakthrough selectivity compared to SION-8P, demonstrating the possibility to rationally tune the separation performance of a single MOF by manipulating the stepwise activation made possible by the MOF's biporous nature.
Databáze: MEDLINE
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