Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling

Claire L. Hobday, Christopher H. Woodall, Matthew J. Lennox, Mungo Frost, Konstantin Kamenev, Tina Düren, Carole A Morrison, Stephen A. Moggach

Research output: Contribution to journalArticle

Abstract

Some porous crystalline solids change their structure upon guest inclusion. Unlocking the potential of these solids for a wide variety of applications requires full characterisation of the response to adsorption and the underlying framework–guest interactions. Here, we introduce an approach to understanding gas uptake in porous metal-organic frameworks (MOFs) by loading liquefied gases at GPa pressures inside the Zn-based framework ZIF-8. An integrated experimental and computational study using high-pressure crystallography, grand canonical Monte Carlo (GCMC) and periodic DFT simulations has revealed six symmetry-independent adsorption sites within the framework and a transition to a high-pressure phase. The cryogenic high-pressure loading method offers a different approach to obtaining atomistic detail on guest molecules. The GCMC simulations provide information on interaction energies of the adsorption sites allowing to classify the sites by energy. DFT calculations reveal the energy barrier of the transition to the high-pressure phase. This combination of techniques provides a holistic approach to understanding both structural and energetic changes upon adsorption in MOFs.
LanguageEnglish
Article number1429
JournalNature Communications
Volume9
Issue number1
DOIs
StatusPublished - 12 Apr 2018

Fingerprint

Crystallography
Adsorption
crystallography
Pressure
adsorption
Discrete Fourier transforms
liquefied gases
Gases
Metals
Liquefied gases
metals
cryogenics
Energy barriers
energy
simulation
Cryogenics
interactions
inclusions
Crystalline materials
symmetry

Cite this

Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling. / Hobday, Claire L.; Woodall, Christopher H.; Lennox, Matthew J.; Frost, Mungo; Kamenev, Konstantin; Düren, Tina; Morrison, Carole A; Moggach, Stephen A.

In: Nature Communications, Vol. 9, No. 1, 1429, 12.04.2018.

Research output: Contribution to journalArticle

Hobday, Claire L. ; Woodall, Christopher H. ; Lennox, Matthew J. ; Frost, Mungo ; Kamenev, Konstantin ; Düren, Tina ; Morrison, Carole A ; Moggach, Stephen A./ Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling. In: Nature Communications. 2018 ; Vol. 9, No. 1.
@article{79ab0a5fac224a36a0eb616f5f931238,
title = "Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling",
abstract = "Some porous crystalline solids change their structure upon guest inclusion. Unlocking the potential of these solids for a wide variety of applications requires full characterisation of the response to adsorption and the underlying framework–guest interactions. Here, we introduce an approach to understanding gas uptake in porous metal-organic frameworks (MOFs) by loading liquefied gases at GPa pressures inside the Zn-based framework ZIF-8. An integrated experimental and computational study using high-pressure crystallography, grand canonical Monte Carlo (GCMC) and periodic DFT simulations has revealed six symmetry-independent adsorption sites within the framework and a transition to a high-pressure phase. The cryogenic high-pressure loading method offers a different approach to obtaining atomistic detail on guest molecules. The GCMC simulations provide information on interaction energies of the adsorption sites allowing to classify the sites by energy. DFT calculations reveal the energy barrier of the transition to the high-pressure phase. This combination of techniques provides a holistic approach to understanding both structural and energetic changes upon adsorption in MOFs.",
author = "Hobday, {Claire L.} and Woodall, {Christopher H.} and Lennox, {Matthew J.} and Mungo Frost and Konstantin Kamenev and Tina D{\"u}ren and Morrison, {Carole A} and Moggach, {Stephen A.}",
year = "2018",
month = "4",
day = "12",
doi = "10.1038/s41467-018-03878-6",
language = "English",
volume = "9",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",
number = "1",

}

TY - JOUR

T1 - Understanding the adsorption process in ZIF-8 using high pressure crystallography and computational modelling

AU - Hobday,Claire L.

AU - Woodall,Christopher H.

AU - Lennox,Matthew J.

AU - Frost,Mungo

AU - Kamenev,Konstantin

AU - Düren,Tina

AU - Morrison,Carole A

AU - Moggach,Stephen A.

PY - 2018/4/12

Y1 - 2018/4/12

N2 - Some porous crystalline solids change their structure upon guest inclusion. Unlocking the potential of these solids for a wide variety of applications requires full characterisation of the response to adsorption and the underlying framework–guest interactions. Here, we introduce an approach to understanding gas uptake in porous metal-organic frameworks (MOFs) by loading liquefied gases at GPa pressures inside the Zn-based framework ZIF-8. An integrated experimental and computational study using high-pressure crystallography, grand canonical Monte Carlo (GCMC) and periodic DFT simulations has revealed six symmetry-independent adsorption sites within the framework and a transition to a high-pressure phase. The cryogenic high-pressure loading method offers a different approach to obtaining atomistic detail on guest molecules. The GCMC simulations provide information on interaction energies of the adsorption sites allowing to classify the sites by energy. DFT calculations reveal the energy barrier of the transition to the high-pressure phase. This combination of techniques provides a holistic approach to understanding both structural and energetic changes upon adsorption in MOFs.

AB - Some porous crystalline solids change their structure upon guest inclusion. Unlocking the potential of these solids for a wide variety of applications requires full characterisation of the response to adsorption and the underlying framework–guest interactions. Here, we introduce an approach to understanding gas uptake in porous metal-organic frameworks (MOFs) by loading liquefied gases at GPa pressures inside the Zn-based framework ZIF-8. An integrated experimental and computational study using high-pressure crystallography, grand canonical Monte Carlo (GCMC) and periodic DFT simulations has revealed six symmetry-independent adsorption sites within the framework and a transition to a high-pressure phase. The cryogenic high-pressure loading method offers a different approach to obtaining atomistic detail on guest molecules. The GCMC simulations provide information on interaction energies of the adsorption sites allowing to classify the sites by energy. DFT calculations reveal the energy barrier of the transition to the high-pressure phase. This combination of techniques provides a holistic approach to understanding both structural and energetic changes upon adsorption in MOFs.

U2 - 10.1038/s41467-018-03878-6

DO - 10.1038/s41467-018-03878-6

M3 - Article

VL - 9

JO - Nature Communications

T2 - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

M1 - 1429

ER -