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Unravelling the origin of enhanced CO<sub>2</sub> selectivity in amine-PIM-1 during mixed gas permeation     
Yazarlar (15)
Carmen Rizzuto
Consiglio Nazionale delle Ricerche (CNR), İtalya
Francesca Nardelli
Consiglio Nazionale delle Ricerche (CNR), İtalya
Marcello Monteleone
Consiglio Nazionale delle Ricerche (CNR), İtalya
Lucia Calucci
Consiglio Nazionale delle Ricerche (CNR), İtalya
C. Grazia Bezzu
Swansea University, İngiltere
Mariolino Carta
Swansea University, İngiltere
Elena Tocci
Consiglio Nazionale delle Ricerche (CNR), İtalya
Elisa Esposito
Consiglio Nazionale delle Ricerche (CNR), İtalya
Giorgio De Luca
Consiglio Nazionale delle Ricerche (CNR), İtalya
Bibiana Comesana-Gandara
Universidad de Valladolid, İspanya
Neil B. Mckeown
University of Edinburgh, İngiltere
Doç. Dr. Bekir SAYGINER Doç. Dr. Bekir SAYGINER
Kırşehir Ahi Evran Üniversitesi, Türkiye
Peter M. Budd
University of Manchester, İngiltere
Johannes C. Jansen
Consiglio Nazionale delle Ricerche (CNR), İtalya
Alessio Fuoco
Consiglio Nazionale delle Ricerche (CNR), İtalya
Devamını Göster
Özet
Previously, it has been reported that amine-PIM-1, a polymer of intrinsic microporosity obtained by reduction of nitrile groups of PIM-1 to primary amine groups, shows enhanced CO 2 selectivity during mixed gas permeation studies with respect to single gas measurements for gas pairs involving CO 2. This distinct and potentially useful behaviour was ascribed to the affinity of CO 2 for the polymer amine groups. Here, we demonstrate that enhanced selectivity originates from both CO 2 physisorption and chemisorption. A combination of 13 C and 15 N solid-state NMR spectroscopic analyses of a CO 2-loaded amine-PIM-1 membrane allowed the identification and quantitative determination of both chemisorbed and physisorbed species and the characterization of polymer-CO 2 interactions. Experiments with 13 C isotopically enriched CO 2 unequivocally demonstrated the conversion of 20% of the NH2 groups into carbamic acids at 298 K and a CO 2 pressure of 1 bar. Chemisorption was supported by the strong heat of CO 2 adsorption for amine-PIM-1 that was estimated as 50 kJ mol-1. Molecular Dynamics simulations with models based on the experimentally determined polymer structure gave a detailed description of intra-and interchain hydrogen bond interactions in amine-PIM-1 after chemisorption, as well as of the effect of chemisorption on polymer porosity and physisorption.
Anahtar Kelimeler
Makale Türü Açık Erişim Özgün Makale
Makale Alt Türü SSCI, AHCI, SCI, SCI-Exp dergilerinde yayınlanan tam makale
Dergi Adı JOURNAL OF MATERIALS CHEMISTRY A
Dergi ISSN 2050-7488 Wos Dergi Scopus Dergi
Dergi Tarandığı Indeksler SCI
Dergi Grubu Q1
Makale Dili Türkçe
Basım Tarihi 01-2025
Cilt No 13
Sayı 23
Sayfalar 12 / 17876
DOI Numarası 10.1039/d4ta08839e
Makale Linki https://doi.org/10.1039/d4ta08839e