Discovering the Active Sites for C3 Separation in MIL-100(Fe) by Using Operando IR Spectroscopy

作者：Wuttke Stefan; Bazin Philippe; Vimont Alexandre; Serre Christian; Seo You Kyong; Hwang Young Kyu; Chang Jong San; Ferey Gerard; Daturi Marco^*

来源：Chemistry - A European Journal, 2012, 18(38): 11959-11967.

DOI：10.1002/chem.201201006

• active sites
• hydrocarbon separation
• IR spectroscopy
• metal-organic frameworks
• IR spectroscopy
• reaction mechanisms

A reducible MIL-100(Fe) metalorganic 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.

• 出版日期2012-9