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

被引：94

作者：

Hulvey, Zeric ^{[1
,2
,3
]}

Lawler, Keith V. ^{[3
]}

Qiao, Zhiwei ^{[4
,5
]}

Zhou, Jian ^{[5
]}

Fairen-Jimenez, David ^{[4
,6
]}

Snurr, Randall Q. ^{[4
]}

Ushakov, Sergey V. ^{[7
,8
]}

Navrotsky, Alexandra ^{[7
,8
]}

Brown, Craig M. ^{[1
,9
]}

Forster, Paul M. ^{[3
]}

机构：

[1] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA

[2] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA

[3] Univ Nevada, Dept Chem, Las Vegas, NV 89154 USA

[4] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA

[5] S China Univ Technol, Guangdong Prov Key Lab Green Chem Prod Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China

[6] Univ Cambridge, Dept Chem Engn & Biotechnol, Cambridge CB2 3RA, England

[7] Univ Calif Davis, Peter A Rock Thermochem Lab, Davis, CA 95616 USA

[8] Univ Calif Davis, NEAT ORU, Davis, CA 95616 USA

[9] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2013年 / 117卷 / 39期

关键词：

METAL-ORGANIC FRAMEWORK; MOLECULAR SIMULATION; POWDER DIFFRACTION; FORCE-FIELD; SEPARATION; CU-3(BTC)(2); HYDROGEN; SITES; SELECTIVITY; SORPTION;

D O I：

10.1021/jp408034u

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A joint experimental and computational study of noble gas adsorption in the metal-organic 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-Clapeyron 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.

引用

页码：20116 / 20126

页数：11

共 48 条

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