In:
ChemPhysChem, Wiley, Vol. 15, No. 9 ( 2014-06-23), p. 1772-1778
Kurzfassung:
Porous aromatic frameworks (PAFs) are novel materials with diamond topology. With the aim of enhancing their CO 2 capture and storage capacity and investigating the effect of nitrogen and/or ‐COOH decorations on CO 2 adsorption in PAFs, a series of N‐containing PAFs were designed based on ab initio results. The interaction energies ( E int ) between CO 2 and each six‐membered ring were calculated at the B2PLYP‐D2/def2‐TZVPP level, then the six‐membered rings with high CO 2 ‐binding affinity were selected and used in the PAFs. To explore the performance of the designed PAFs, the CO 2 uptake, selectivity of CO 2 over CH 4 , H 2 , and N 2 , and the E int value of CO 2 in PAFs were investigated by using grand canonical Monte Carlo (GCMC) simulations and ab initio calculations. This work shows that pyridine with one nitrogen atom can provide a strong physisorption site for CO 2 , whereas more nitrogen atoms in heterocycles will reduce the interaction, especially at relatively low pressure. PAFs with COOH groups show high CO 2 capacity. Our work provides an efficient way to understand the adsorption mechanism and a supplemental approach to experimental work.
Materialart:
Online-Ressource
ISSN:
1439-4235
,
1439-7641
DOI:
10.1002/cphc.201400064
Sprache:
Englisch
Verlag:
Wiley
Publikationsdatum:
2014
ZDB Id:
2025223-7
ZDB Id:
2021755-9
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