Noble gas adsorption in copper trimesate, HKUST-1: An experimental and computational study

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

doi:10.1021/jp408034u

Noble gas adsorption in copper trimesate, HKUST-1: An experimental and computational study

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

Research output: Contribution to journal › Article › peer-review

93 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	20116-20126
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	117
Issue number	39
DOIs	https://doi.org/10.1021/jp408034u
State	Published - Oct 3 2013
Externally published	Yes

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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10.1021/jp408034u

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@article{9ec37bf4a96a4d59b16fc30315152462,

title = "Noble gas adsorption in copper trimesate, HKUST-1: An experimental and computational study",

abstract = "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.",

author = "Zeric Hulvey and Lawler, {Keith V.} and Zhiwei Qiao and Jian Zhou and David Fairen-Jimenez and Snurr, {Randall Q.} and Ushakov, {Sergey V.} and Alexandra Navrotsky and Brown, {Craig M.} and Forster, {Paul M.}",

year = "2013",

month = oct,

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doi = "10.1021/jp408034u",

language = "English (US)",

volume = "117",

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journal = "Journal of Physical Chemistry C",

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publisher = "American Chemical Society",

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TY - JOUR

T1 - Noble gas adsorption in copper trimesate, HKUST-1

T2 - An experimental and computational study

AU - Hulvey, Zeric

AU - Lawler, Keith V.

AU - Qiao, Zhiwei

AU - Zhou, Jian

AU - Fairen-Jimenez, David

AU - Snurr, Randall Q.

AU - Ushakov, Sergey V.

AU - Navrotsky, Alexandra

AU - Brown, Craig M.

AU - Forster, Paul M.

PY - 2013/10/3

Y1 - 2013/10/3

N2 - 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.

AB - 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.

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DO - 10.1021/jp408034u

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JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

IS - 39

ER -

Noble gas adsorption in copper trimesate, HKUST-1: An experimental and computational study

Abstract

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