Separation of Aromatic Hydrocarbons in Porous Materials

Karam B. Idrees; Zhao Li; Haomiao Xie; Kent O. Kirlikovali; Masoud Kazem-Rostami; Xingjie Wang; Xijun Wang; Tzu Yi Tai; Timur Islamoglu; J. Fraser Stoddart; Randall Q. Snurr; Omar K. Farha

doi:10.1021/jacs.2c03114

Separation of Aromatic Hydrocarbons in Porous Materials

Karam B. Idrees, Zhao Li, Haomiao Xie, Kent O. Kirlikovali, Masoud Kazem-Rostami, Xingjie Wang, Xijun Wang, Tzu Yi Tai, Timur Islamoglu, J. Fraser Stoddart, Randall Q. Snurr, Omar K. Farha^*

^*Corresponding author for this work

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

76 Scopus citations

Abstract

Industrial-scale thermal separation processes have contributed greatly to the rise in carbon dioxide emissions. Porous materials, such as metal-organic frameworks (MOFs), can potentially reduce these emissions by achieving nonthermal chemical separations through the physical adsorption of targeted species with high selectivity. Here, we report the synthesis of the channel-based MOFs NU-2000 and NU-2001, which are constructed from three-dimensional (3D) linkers, to separate the industrially relevant xylene isomers under ambient conditions by leveraging sub-Ångstrom differences in the sizes of each isomer. While the rotation of two-dimensional (2D) linkers in MOFs often affords changes in pore apertures and pore sizes that are substantial enough to hinder separation efficiency, increasing the linker dimensionality from 2D to three-dimensional (3D) enables precise control of the MOF pore size and aperture regardless of the linker orientation, establishing this design principle as a broadly applicable strategy.

Original language	English (US)
Pages (from-to)	12212-12218
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	144
Issue number	27
DOIs	https://doi.org/10.1021/jacs.2c03114
State	Published - Jul 13 2022

Funding

O.K.F. and R.Q.S. gratefully acknowledge research support from the U.S. Department of Energy (DOE) Office of Science, Basic Energy Sciences Program for separation studies and modeling (DE-FG02-08ER15967), and O.K.F. thanks the Defense Threat Reduction Agency for support of the MOF synthesis (HDTRA1-19-1-0007). K.O.K. acknowledges support from the IIN Postdoctoral Fellowship and the Northwestern University International Institute of Nanotechnology. This work made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR1720139) at the Materials Research Center; the Keck Foundation; the International Institute for Nanotechnology (IIN); and the State of Illinois through the IIN. This work made use of the IMSERC at Northwestern University, which has received support from the NSF (CHE-1048773 and DMR0521267); the SHyNE Resource (NSF NNCI-1542205); the State of Illinois, and the IIN. This research was partly supported by the computational resources provided for the Quest high-performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. Z.L. acknowledges support from a Data Science Fellowship via the Northwestern Institute on Complex Systems. Z.L. also gratefully thanks Professor David Dubbeldam for the helpful discussion on the minimization calculations in RASPA and simulation files for MIL-53.

Keywords

flexibility
metal-organic frameworks
separation
xylenes

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/jacs.2c03114

Cite this

@article{9c3dd71b2c2f48088d23fd5457655429,

title = "Separation of Aromatic Hydrocarbons in Porous Materials",

abstract = "Industrial-scale thermal separation processes have contributed greatly to the rise in carbon dioxide emissions. Porous materials, such as metal-organic frameworks (MOFs), can potentially reduce these emissions by achieving nonthermal chemical separations through the physical adsorption of targeted species with high selectivity. Here, we report the synthesis of the channel-based MOFs NU-2000 and NU-2001, which are constructed from three-dimensional (3D) linkers, to separate the industrially relevant xylene isomers under ambient conditions by leveraging sub-{\AA}ngstrom differences in the sizes of each isomer. While the rotation of two-dimensional (2D) linkers in MOFs often affords changes in pore apertures and pore sizes that are substantial enough to hinder separation efficiency, increasing the linker dimensionality from 2D to three-dimensional (3D) enables precise control of the MOF pore size and aperture regardless of the linker orientation, establishing this design principle as a broadly applicable strategy.",

keywords = "flexibility, metal-organic frameworks, separation, xylenes",

author = "Idrees, {Karam B.} and Zhao Li and Haomiao Xie and Kirlikovali, {Kent O.} and Masoud Kazem-Rostami and Xingjie Wang and Xijun Wang and Tai, {Tzu Yi} and Timur Islamoglu and Stoddart, {J. Fraser} and Snurr, {Randall Q.} and Farha, {Omar K.}",

note = "Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = jul,

day = "13",

doi = "10.1021/jacs.2c03114",

language = "English (US)",

volume = "144",

pages = "12212--12218",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "27",

}

TY - JOUR

T1 - Separation of Aromatic Hydrocarbons in Porous Materials

AU - Idrees, Karam B.

AU - Li, Zhao

AU - Xie, Haomiao

AU - Kirlikovali, Kent O.

AU - Kazem-Rostami, Masoud

AU - Wang, Xingjie

AU - Wang, Xijun

AU - Tai, Tzu Yi

AU - Islamoglu, Timur

AU - Stoddart, J. Fraser

AU - Snurr, Randall Q.

AU - Farha, Omar K.

PY - 2022/7/13

Y1 - 2022/7/13

N2 - Industrial-scale thermal separation processes have contributed greatly to the rise in carbon dioxide emissions. Porous materials, such as metal-organic frameworks (MOFs), can potentially reduce these emissions by achieving nonthermal chemical separations through the physical adsorption of targeted species with high selectivity. Here, we report the synthesis of the channel-based MOFs NU-2000 and NU-2001, which are constructed from three-dimensional (3D) linkers, to separate the industrially relevant xylene isomers under ambient conditions by leveraging sub-Ångstrom differences in the sizes of each isomer. While the rotation of two-dimensional (2D) linkers in MOFs often affords changes in pore apertures and pore sizes that are substantial enough to hinder separation efficiency, increasing the linker dimensionality from 2D to three-dimensional (3D) enables precise control of the MOF pore size and aperture regardless of the linker orientation, establishing this design principle as a broadly applicable strategy.

AB - Industrial-scale thermal separation processes have contributed greatly to the rise in carbon dioxide emissions. Porous materials, such as metal-organic frameworks (MOFs), can potentially reduce these emissions by achieving nonthermal chemical separations through the physical adsorption of targeted species with high selectivity. Here, we report the synthesis of the channel-based MOFs NU-2000 and NU-2001, which are constructed from three-dimensional (3D) linkers, to separate the industrially relevant xylene isomers under ambient conditions by leveraging sub-Ångstrom differences in the sizes of each isomer. While the rotation of two-dimensional (2D) linkers in MOFs often affords changes in pore apertures and pore sizes that are substantial enough to hinder separation efficiency, increasing the linker dimensionality from 2D to three-dimensional (3D) enables precise control of the MOF pore size and aperture regardless of the linker orientation, establishing this design principle as a broadly applicable strategy.

KW - flexibility

KW - metal-organic frameworks

KW - separation

KW - xylenes

UR - http://www.scopus.com/inward/record.url?scp=85134427012&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85134427012&partnerID=8YFLogxK

U2 - 10.1021/jacs.2c03114

DO - 10.1021/jacs.2c03114

M3 - Article

C2 - 35786875

AN - SCOPUS:85134427012

SN - 0002-7863

VL - 144

SP - 12212

EP - 12218

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 27

ER -

Separation of Aromatic Hydrocarbons in Porous Materials

Abstract

Funding

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

CCDC 2151358: Experimental Crystal Structure Determination

CCDC 2151356: Experimental Crystal Structure Determination

CCDC 2151357: Experimental Crystal Structure Determination

Cite this

Separation of Aromatic Hydrocarbons in Porous Materials

Abstract

Funding

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Datasets

CCDC 2151358: Experimental Crystal Structure Determination

CCDC 2151356: Experimental Crystal Structure Determination

CCDC 2151357: Experimental Crystal Structure Determination

Cite this