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The accessibility of nitrogen sites makes a difference in selective CO2 adsorption of a family of isostructural metal-organic frameworksElectronic supplementary information (ESI) available: PXRD patterns (Fig. S1-S3), TGA (Fig. S4), gas sorption isotherms (Fig. S5-S7), schematic of the breakthrough apparatus (Fig. S8), FTIR spectra (Fig. S9-S11), 1H and 13C NMR (Fig. S12), comparison of the textural properties of ZJNU-43a, ZJNU-44a and ZJNU-45 (Table S1), single-site Langmuir fit parameters (Tab
Erscheinungsjahr
2015-09
Link zum Volltext
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
By using three rigid diisophthalate organic linkers incorporating different numbers and orientations of Lewis basic nitrogen atoms into the spacers between two terminal isophthalate moieties, namely, 5,5′-(quinoline-5,8-diyl)-diisophthalate, 5,5′-(isoquinoline-5,8-diyl)-diisophthalate, and 5,5′-(quinoxaline-5,8-diyl)-diisophthalate, a family of isostructural copper-based metal-organic frameworks,
ZJNU-43
,
ZJNU-44
and
ZJNU-45
, were successfully solvothermally synthesized and structurally characterized by single-crystal X-ray diffraction. The three MOFs, after activation, exhibited almost the same porosities but distinctly different CO
2
adsorption properties. At room temperature and 1 atm, the adsorption capacities for CO
2
reached 103, 116 and 107 cm
3
(STP) g
−1
for
ZJNU-43a
,
ZJNU-44a
and
ZJNU-45a
, respectively. Furthermore, Ideal Adsorbed Solution Theory (IAST) and simulated breakthrough analyses indicated that
ZJNU-44a
bearing much more easily accessible nitrogen sites is the best among the three MOFs for the separation of the following two binary gas mixtures at 296 K,
i.e.
, 50/50 CO
2
/CH
4
and 15/85 CO
2
/N
2
gas mixtures, indicating that the accessibility of nitrogen sites plays a much more crucial role, which is further confirmed by comprehensive quantum chemical calculations. The work demonstrates that the CO
2
adsorption properties of MOFs depend not only on the number of Lewis basic nitrogen sites but also more importantly on their accessibility.
Three isostructural metal-organic frameworks exhibit different CO
2
adsorption properties depending on the number and orientation of nitrogen sites in the frameworks, and the accessibility of nitrogen sites plays a much more crucial role in enhancing CO
2
adsorption.
Sprache
Englisch
Identifikatoren
ISSN: 2050-7488
eISSN: 2050-7496
DOI: 10.1039/c5ta05481h
Titel-ID: cdi_rsc_primary_c5ta05481h
Format
–
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