Noble Gas Adsorption in Copper Trimesate, HKUST-1: An Experimental and Computational Study

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• 作者：Zeric Hulvey ; Keith V. Lawler ; Zhiwei Qiao ; Jian Zhou ; David Fairen-Jimenez ; Randall Q. Snurr ; Sergey V. Ushakov ; Alexandra Navrotsky ; Craig M. Brown ; Paul M. Forster
• 刊名：Journal of Physical Chemistry C
• 出版年：2013
• 出版时间：October 3, 2013
• 年：2013
• 卷：117
• 期：39
• 页码：20116-20126
• 全文大小：574K
• 年卷期：v.117,no.39(October 3, 2013)
• ISSN：1932-7455

文摘

A joint experimental and computational study of noble gas adsorption in the metal鈥搊rganic framework (MOF) material HKUST-1 has been carried out. Using a standard gas adsorption analyzer fitted with a cryostat, isotherms were measured for Xe, Kr, Ar, and Ne at optimum temperatures for the determination of loading-dependent heats of adsorption using the Clausius鈥揅lapeyron equation. Direct calorimetric measurements for Kr and Xe adsorption provide comparable heats of adsorption. A detailed analysis of the experimental data alongside complementary grand canonical Monte Carlo (GCMC) simulations led to the conclusion that the strongest binding for noble gases occurs in and around the small tetrahedral pockets and not at the accessible Cu(II) sites in the structure. Synchrotron X-ray and neutron powder diffraction experiments with in situ gas loading confirm the assignment of preferred binding sites inferred from the adsorption measurements and simulations.