Details

Autor(en) / Beteiligte

• Song, Chengling
• Hu, Jiayi
• Ling, Yajing
• Feng, Yunlong
• Chen, De-Li
• He, Yabing

Titel

Merging open metal sites and Lewis basic sites in a NbO-type metal-organic framework for improved C2H2/CH4 and CO2/CH4 separationElectronic supplementary information (ESI) available: PXRD pattern (Fig. S1), TGA (Fig. S2), N2 adsorption-desorption isotherm (Fig. S3), BET and Langmuir plots (Fig. S4), FTIR spectra (Fig. S5), NMR spectra (Fig. S6), crystal data and structure refinement for ZJNU-47 (Table S1). CCDC 1056733. For ESI and crystallographic data in CIF or other electronic format see DOI:

Erscheinungsjahr

2015-08

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• A new three-dimensional NbO-type porous metal-organic framework ZJNU-47 was synthesized via a solvothermal reaction of Cu(NO 3 ) 2 ·3H 2 O and a Lewis basic nitrogen donor site-rich tetracarboxylate, namely, 5,5′-(pyridazine-3,6-diyl)-diisophthalate, and the structure was characterized by single-crystal X-ray diffraction to be isostructural with NOTT-101 . With the synergistic effect of open metal sites, Lewis basic sites and a suitable pore space, the MOF material ZJNU-47a after activation can take up a large amount of C 2 H 2 and CO 2 . The gravimetric C 2 H 2 uptake of 214 cm 3 (STP) g −1 at room temperature and 1 atm is the highest among all reported MOFs to date, and the gravimetric CO 2 uptake of 108 cm 3 (STP) g −1 is also among the highest reported for MOFs. Compared to the isostructural MOF NOTT-101a , ZJNU-47a exhibits a significant increase in C 2 H 2 and CO 2 uptake and thus improved C 2 H 2 /CH 4 and CO 2 /CH 4 separations. Significantly, comprehensive DFT studies of C 2 H 2 and CO 2 adsorption have revealed that the open nitrogen donor sites are comparable and even superior to open metal sites regarding the adsorption sites. This work demonstrated that the simultaneous introduction of Lewis basic nitrogen donor sites and Lewis acidic metal sites into the framework is a promising approach to improve the gas sorption toward CO 2 and C 2 H 2 and thus to produce materials possessing enhanced C 2 H 2 /CH 4 and CO 2 /CH 4 separation performance. A new NbO-type metal-organic framework ZJNU-47a incorporating Lewis acidic copper sites and Lewis basic nitrogen donor sites exhibits better performance than the isostructural NOTT-101a in the separation of C 2 H 2 /CH 4 and CO 2 /CH 4 gas mixtures at room temperature.