Metal−Organic Frameworks Impregnated with Magnesium-Decorated Fullerenes for Methane and Hydrogen Storage

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• 作者：Aaron W. Thornton ; Kate M. Nairn ; James M. Hill ; Anita J. Hill ; Matthew R. Hill
• 刊名：Journal of the American Chemical Society
• 出版年：2009
• 出版时间：August 5, 2009
• 年：2009
• 卷：131
• 期：30
• 页码：10662-10669
• 全文大小：528K
• 年卷期：v.131,no.30(August 5, 2009)
• ISSN：1520-5126

文摘

A new concept is described for methane and hydrogen storage materials involving the incorporation of magnesium-decorated fullerenes within metal−organic frameworks (MOFs). The system is modeled using a novel approach underpinned by surface potential energies developed from Lennard-Jones parameters. Impregnation of MOF pores with magnesium-decorated Mg₁₀C₆₀ fullerenes, denoted as Mg−C₆₀@MOF, places exposed metal sites with high heats of gas adsorption into intimate contact with large surface area MOF structures. Perhaps surprisingly, given the void space occupied by C₆₀, this impregnation delivers remarkable gas uptake, according to our modeling, which predicts exceptional performance for the Mg−C₆₀@MOF family of materials. These predictions include a volumetric methane uptake of 265 v/v, the highest reported value for any material, which significantly exceeds the U.S. Department of Energy target of 180 v/v. We also predict a very high hydrogen adsorption enthalpy of 11 kJ mol⁻¹ with relatively little decrease as a function of H₂ filling. This value is close to the calculated optimum value of 15.1 kJ mol⁻¹ and is achieved concurrently with saturation hydrogen uptake in large amounts at pressures under 10 atm.