N/S-Heterocyclic Contaminant Removal from Fuels by the Mesoporous Metal鈥揙rganic Framework MIL-100: The Role of the Metal Ion

详细信息    查看全文

• 作者：Ben Van de Voorde ; Mohammed Boulhout ; Frederik Vermoortele ; Patricia Horcajada ; Denise Cunha ; Ji Sun Lee ; Jong-San Chang ; Emma Gibson ; Marco Daturi ; Jean-Claude Lavalley ; Alexandre Vimont ; Isabelle Beurroies ; Dirk E. De Vos
• 刊名：The Journal of the American Chemical Society
• 出版年：2013
• 出版时间：July 3, 2013
• 年：2013
• 卷：135
• 期：26
• 页码：9849-9856
• 全文大小：372K
• 年卷期：v.135,no.26(July 3, 2013)
• ISSN：1520-5126

文摘

The influence of the metal ion in the mesoporous metal trimesate MIL-100(Al³⁺, Cr³⁺, Fe³⁺, V³⁺) on the adsorptive removal of N/S-heterocyclic molecules from fuels has been investigated by combining isotherms for adsorption from a model fuel solution with microcalorimetric and IR spectroscopic characterizations. The results show a clear influence of the different metals (Al, Fe, Cr, V) on the affinity for the heterocyclic compounds, on the integral adsorption enthalpies, and on the uptake capacities. Among several factors, the availability of coordinatively unsaturated sites and the presence of basic sites next to the coordinative vacancies are important factors contributing to the observed affinity differences for N-heterocyclic compounds. These trends were deduced from IR spectroscopic observation of adsorbed indole molecules, which can be chemisorbed coordinatively or by formation of hydrogen bonded species. On the basis of our results we are able to propose an optimized adsorbent for the deep and selective removal of nitrogen contaminants out of fuel feeds, namely MIL-100(V).