Maqola

Microporous Metal–Organic Framework Stabilized by Balanced Multiple Host–Couteranion Hydrogen-Bonding Interactions for High-Density CO<sub>2</sub> Capture at Ambient Conditions

Yingxiang YeCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaShunshun XiongInstitute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan 621900, People’s Republic of ChinaXiaonan WuInstitute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan 621900, People’s Republic of ChinaLiuqin ZhangCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaZiyin LiCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaLihua WangCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaXiuling MaCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaQian‐Huo ChenCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaZhangjing ZhangCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of ChinaShengchang XiangCollege of Chemistry and Chemical Engineering, Fujian Provincial Key Laboratory of Polymer Materials, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, People’s Republic of China

2015en

ABI

Annotatsiya

Microporous metal organic frameworks (MOFs) show promising application in several fields, but they often suffer from the weak robustness and stability after the removal of guest molecules. Here, three isostructural cationic metal-organic frameworks {[(Cu4Cl)(cpt)4(H2O)4]·3X·4DMAc·CH3OH·5H2O} (FJU-14, X = NO3, ClO4, BF4; DMAc = N,N'-dimethylacetamide) containing two types of polyhedral nanocages, one octahedron, and another tetrahedron have been synthesized from bifunctional organic ligands 4-(4H-1,2,4-triazol-4-yl) benzoic acid (Hcpt) and various copper salts. The series of MOFs FJU-14 are demonstrated as the first examples of the isostructural MOFs whose robustness, thermal stability, and CO2 capacity can be greatly improved via rational modulation of counteranions in the tetrahedral cages. The activated FJU-14-BF4-a containing BF4(-) anion can take CO2 of 95.8 cm(3) cm(-3) at ambient conditions with an adsorption enthalpy only of 18.8 kJ mol(-1). The trapped CO2 density of 0.955 g cm(-3) is the highest value among the reported MOFs. Dynamic fixed bed breakthrough experiments indicate that the separation of CO2/N2 mixture gases through a column packed with FJU-14-BF4-a solid can be efficiently achieved. The improved robustness and thermal stability for FJU-14-BF4-a can be attributed to the balanced multiple hydrogen-bonding interactions (MHBIs) between the BF4(-) counteranion and the cationic skeleton, while the high-density and low-enthalpy CO2 capture on FJU-14-BF4-a can be assigned to the multiple-point interactions between the adsorbate molecules and the framework as well as with its counteranions, as proved by single-crystal structures of the guest-free and CO2-loaded FJU-14-BF4-a samples.

Hali tarjima qilinmagan

Identifikatorlar

DOI: 10.1021/acs.inorgchem.5b02316

Iqtiboslar va manbalar

3 ta iqtibos0 ta foydalanilgan manba

Koʻrsatkichlar — AkademScholar