Development of Heterometallic Annular Tetranuclear Clusters in Metal-Organic Frameworks for Methane Purification and Storage.
Journal:
Chem & bio engineering
Published Date:
Mar 15, 2024
Abstract
Annular tetranuclear cluster based metal-organic frameworks (MOFs) have displayed unique advantages in gas adsorption and separation due to their highly connected robust architectures. Herein, two novel heterometallic tetranuclear motifs, [YCd(μ-O)(COO)(HO)] and [YIn(μ-O)(μ-O)(COO)(HO)], were successfully explored, which were further extended by 1,3,5-tris(4-carboxyphenyl)benzene (HBTB) tritopic linker to give isostructural MOFs (SNNU-326 and -327). SNNU-326 and -327 both exhibit the abilities to remove impurities (C-hydrocarbons and CO) in natural gas (NG) and excellent CH storage capacities at high pressures. SNNU-326 shows better CH purification and storage performance than SNNU-327 owing to different framework charges, in which only one counter ion is needed in SNNU-326 but two of them are necessary for SNNU-327, thus resulting in an obvious decrease of surface area. Dynamic breakthrough experiments demonstrate that SNNU-326 can effectively separate CH from equimolar CH/CH, CH/CH, CH/CH, and CO/CH mixtures with breakthrough interval times of about 40.6, 35.1, 54.2, and 10.2 min g (273 K, 1 bar, 2 mL min), respectively. At the same time, SNNU-326 exhibits excellent CH storage capability with total and working uptakes of 154.3 cm (STP) cm (80 bar) and 103.4 cm (STP) cm (5-65 bar) at 273 K on account of the collaborative impacts of adequate apertures, high surface areas, and multiple open metal sites.
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