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1.
ACS Appl Mater Interfaces ; 16(5): 6579-6588, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38275141

RESUMO

Purifying C2H6/C3H8 from a ternary natural gas mixture through adsorption separation is an important but challenging process in the petrochemical industry. To address this challenge, the industry is exploring effective strategies for designing high-performance adsorbents. In this study, we present two metal-organic frameworks (MOFs), DMOF-TF and DMOF-(CF3)2, which have fluorinated pores obtained by substituting linker ligands in the host material. This pore engineering strategy not only provides suitable pore confinement but also enhances the adsorption capacities for C2H6/C3H8 by providing additional binding sites. Theoretical calculations and transient breakthrough experiments show that the introduction of F atoms not only improves the efficiency of natural gas separation but also provides multiple adsorption sites for C2H6/C3H8-framework interactions.

2.
Angew Chem Int Ed Engl ; 61(26): e202201766, 2022 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-35313055

RESUMO

The design and creation of soft porous crystals combining regularity and flexibility may promote potential applications for gas storage and separation due to their deformable framework's responsiveness to external stimuli. The flexibility of metal-organic frameworks (MOFs) relies on alterable degrees of freedom that are mainly provided by organic linkers or the junctions linking organic and inorganic building units. Herein, we report a new dynamic MOF whose flexibility originates from an unprecedented tailorable Mn8 O38 -cluster and shows simultaneous coordination geometry changes and ligand migration that are reversibly driven by guest exchange. This provides an extra degree of freedom to the framework's deformation, resulting in three-dimensional variations in the framework that subtly respond to varied aromatic molecules. The gas adsorption behavior of this flexible MOF was evaluated, and the selective separation of light hydrocarbons and Freon gases is achieved.

3.
Inorg Chem ; 60(12): 8456-8460, 2021 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-34085808

RESUMO

A flexible and robust microporous copper(II) metal-organic framework (MOF) based on a methyl-functionalized ligand, namely, [Cu3(µ3-OH)2(L)2(DMF)] (LIFM-ZZ-1; L = 2,2'-dimethyl-4,4'-biphenyldicarboxylic acid and DMF = N,N-dimethylformamide), was constructed. Its sorption performance for the separation of CH4, C2H6, and C3H8 was investigated. LIFM-ZZ-1 showed a breathing behavior that led to a transition between large- and narrow-pore states. The sample also showed outstanding water stability. Gas adsorption experiments revealed that desolvated LIFM-ZZ-1 exhibited higher adsorption capacities for C2H6 and C3H8 (2.80 and 4.06 mmol·g-1) than for CH4 (0.39 mmol·g-1) at 298 K and 1 bar. Breakthrough experiments showed that a CH4/C2H6/C3H8 mixture was completely separated at 298 K, demonstrating the promising potential applications of this material for separating low contents of C2/C3 hydrocarbons from natural gas.

4.
Chemistry ; 23(15): 3542-3547, 2017 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-28094459

RESUMO

Two analogous M4 L4 -type tetrahedral cages (smaller: MOC-19; larger: MOC-22) were synthesized and investigated for their interactions with the anticancer drug 5-fluoracil (5-FU) by NMR spectroscopy, high-resolution electrospray-ionization mass spectrometry (HR-ESI-MS), and molecular simulation. The cage's size and window are of importance for the host-guest binding, and consequently the smaller MOC-19 with a more suitable size of cavity window was found to have much stronger hydrogen-bond interactions with 5-FU. The porous nanoparticles of MOC-19 exhibited outstanding behavior for the controlled release of 5-FU in a simulated human body with liquid phosphate-buffered saline solution.


Assuntos
Antineoplásicos/administração & dosagem , Preparações de Ação Retardada/química , Fluoruracila/administração & dosagem , Estruturas Metalorgânicas/química , Antineoplásicos/química , Fluoruracila/química , Ligação de Hidrogênio , Espectroscopia de Ressonância Magnética , Modelos Moleculares , Nanopartículas/química , Tamanho da Partícula , Porosidade , Espectrometria de Massas por Ionização por Electrospray
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