From Molecules to Materials: Computational Design of N‐Containing Porous Aromatic Frameworks for CO2 Capture. Issue 9 (23rd June 2014)

• Record Type: Journal Article
• Authors: Li, Wenliang; Shi, Haijie; Zhang, Jingping
• Is Part Of: Chemphyschem. Volume 15:Issue 9(2014)
• Page Start: 1772
• Page End: 1778
• Publication Date: 2014-06-23
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.05
• DOI: 10.1002/cphc.201400064
• Languages: English
• ISSNs: 1439-4235

Abstract

<abstract abstract-type="main" xml:lang="en"> <title>Abstract</title> <p>Porous aromatic frameworks (PAFs) are novel materials with diamond topology. With the aim of enhancing their CO₂ capture and storage capacity and investigating the effect of nitrogen and/or ‐COOH decorations on CO₂ adsorption in PAFs, a series of N‐containing PAFs were designed based on ab initio results. The interaction energies (<italic>E</italic>_int) between CO₂ and each six‐membered ring were calculated at the B2PLYP‐D2/def2‐TZVPP level, then the six‐membered rings with high CO₂‐binding affinity were selected and used in the PAFs. To explore the performance of the designed PAFs, the CO₂ uptake, selectivity of CO₂ over CH₄, H₂, and N₂, and the <italic>E</italic>_int value of CO₂ 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 CO₂, whereas more nitrogen atoms in heterocycles will reduce the interaction, especially at relatively low pressure. PAFs with COOH groups show high CO₂ capacity. Our work provides an efficient way to understand the adsorption mechanism and a supplemental approach to experimental work.</p> </abstract>