TY - JOUR
T1 - Discovering the active sites for C3 separation in MIL-100(Fe) by using operando IR spectroscopy
AU - Wuttke, Stefan
AU - Bazin, Philippe
AU - Vimont, Alexandre
AU - Serre, Christian
AU - Seo, You Kyong
AU - Hwang, Young Kyu
AU - Chang, Jong San
AU - Férey, Gérard
AU - Daturi, Marco
PY - 2012/9/17
Y1 - 2012/9/17
N2 - A reducible MIL-100(Fe) metal-organic framework (MOF) was investigated for the separation of a propane/propene mixture. An operando methodology was applied (for the first time in the case of a MOF) in order to shed light on the separation mechanism. Breakthrough curves were obtained as in traditional separation column experiments, but monitoring the material surface online, thus providing evidences on the adsorption sites. The qualitative and quantitative analyses of FeII and, to some extent, FeIII sites were possible, upon different activation protocols. Moreover, it was possible to identify the nature and the role of the active sites in the separation process by selective poisoning of one family of sites: it was clearly evidenced that the unsaturated FeII sites are mainly responsible for the separation effect of the propane/propene mixture, thanks to their affinity for the unsaturated bonds, such as the C=C entities in propene. The activity of the highly concentrated FeIII sites was also highlighted.
AB - A reducible MIL-100(Fe) metal-organic framework (MOF) was investigated for the separation of a propane/propene mixture. An operando methodology was applied (for the first time in the case of a MOF) in order to shed light on the separation mechanism. Breakthrough curves were obtained as in traditional separation column experiments, but monitoring the material surface online, thus providing evidences on the adsorption sites. The qualitative and quantitative analyses of FeII and, to some extent, FeIII sites were possible, upon different activation protocols. Moreover, it was possible to identify the nature and the role of the active sites in the separation process by selective poisoning of one family of sites: it was clearly evidenced that the unsaturated FeII sites are mainly responsible for the separation effect of the propane/propene mixture, thanks to their affinity for the unsaturated bonds, such as the C=C entities in propene. The activity of the highly concentrated FeIII sites was also highlighted.
KW - active sites
KW - hydrocarbon separation
KW - IR spectroscopy
KW - metal-organic frameworks
KW - reaction mechanisms
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U2 - 10.1002/chem.201201006
DO - 10.1002/chem.201201006
M3 - Article
C2 - 22890853
AN - SCOPUS:84866258815
SN - 0947-6539
VL - 18
SP - 11959
EP - 11967
JO - Chemistry - A European Journal
JF - Chemistry - A European Journal
IS - 38
ER -