Adsorptive separation of xenon/krypton mixtures using ligand controls in a zirconium-based metal-organic framework

Seung Joon Lee; Seongwoo Kim; Eun Jung Kim; Min Kim; Youn Sang Bae

doi:10.1016/j.cej.2017.10.155

Adsorptive separation of xenon/krypton mixtures using ligand controls in a zirconium-based metal-organic framework

Seung Joon Lee, Seongwoo Kim, Eun Jung Kim, Min Kim, Youn Sang Bae

Department of Chemical and Biomolecular Engineering

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

50 Citations (Scopus)

Abstract

A Zr-based metal-organic framework (MOF), UiO-66, is considered to be one of the most stable MOFs and has recently been shown to be a good candidate for adsorptive separation of Xe/Kr mixtures. Since the ability to impart chemical functionalities is an attractive characteristic of MOFs, herein, we prepared a series of functionalized UiO-66 materials (UiO-66-NH₂, UiO-66-(OMe)₂, UiO-66-NH₂(OMe)₂, and UiO-66-F₄) by incorporating several polar functionalities into UiO-66. We found that series of electron-rich and electron-deficient UiO-66 materials have stronger interactions with Xe and Kr atoms than pristine UiO-66. We also found that Xe/Kr selectivity increases with the electron density of the ligand. Although there was a reduction in surface area, UiO-66-NH₂(OMe)₂ exhibited the highest Xe/Kr Henry's constant ratio (14.4), possibly due to having the highest electron density as well as an unsymmetrical arrangement of functional groups of the ligands. Furthermore, the breakthrough experiments show that UiO-66-NH₂(OMe)₂ can effectively separate Xe from Kr under dynamic mixture conditions and can be easily regenerated under a mild regeneration condition.

Original language	English
Pages (from-to)	345-351
Number of pages	7
Journal	Chemical Engineering Journal
Volume	335
DOIs	https://doi.org/10.1016/j.cej.2017.10.155
Publication status	Published - 2018 Mar 1

Bibliographical note

Funding Information:
This work was supported in part by the National Research Foundation of Korea under Grant ( NRF-2016R1A2B4014256 for S.-J.L. and Y.-S.B.; the Science Research Center NRF-2016R1A5A1009405 for S.K. and M.K.). This work was also supported by the National Institute of Supercomputing and Network/ Korea Institute of Science and Technology Information with supercomputing resources including technical support ( KSC-2015-C1-016 ). Appendix A

Publisher Copyright:
© 2017 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Chemistry(all)
Environmental Chemistry
Chemical Engineering(all)
Industrial and Manufacturing Engineering

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10.1016/j.cej.2017.10.155

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@article{f527068f719f490692741d0bda00a121,

title = "Adsorptive separation of xenon/krypton mixtures using ligand controls in a zirconium-based metal-organic framework",

abstract = "A Zr-based metal-organic framework (MOF), UiO-66, is considered to be one of the most stable MOFs and has recently been shown to be a good candidate for adsorptive separation of Xe/Kr mixtures. Since the ability to impart chemical functionalities is an attractive characteristic of MOFs, herein, we prepared a series of functionalized UiO-66 materials (UiO-66-NH2, UiO-66-(OMe)2, UiO-66-NH2(OMe)2, and UiO-66-F4) by incorporating several polar functionalities into UiO-66. We found that series of electron-rich and electron-deficient UiO-66 materials have stronger interactions with Xe and Kr atoms than pristine UiO-66. We also found that Xe/Kr selectivity increases with the electron density of the ligand. Although there was a reduction in surface area, UiO-66-NH2(OMe)2 exhibited the highest Xe/Kr Henry's constant ratio (14.4), possibly due to having the highest electron density as well as an unsymmetrical arrangement of functional groups of the ligands. Furthermore, the breakthrough experiments show that UiO-66-NH2(OMe)2 can effectively separate Xe from Kr under dynamic mixture conditions and can be easily regenerated under a mild regeneration condition.",

author = "Lee, {Seung Joon} and Seongwoo Kim and Kim, {Eun Jung} and Min Kim and Bae, {Youn Sang}",

note = "Funding Information: This work was supported in part by the National Research Foundation of Korea under Grant ( NRF-2016R1A2B4014256 for S.-J.L. and Y.-S.B.; the Science Research Center NRF-2016R1A5A1009405 for S.K. and M.K.). This work was also supported by the National Institute of Supercomputing and Network/ Korea Institute of Science and Technology Information with supercomputing resources including technical support ( KSC-2015-C1-016 ). Appendix A Publisher Copyright: {\textcopyright} 2017 Elsevier B.V.",

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AU - Lee, Seung Joon

AU - Kim, Seongwoo

AU - Kim, Eun Jung

AU - Kim, Min

AU - Bae, Youn Sang

N1 - Funding Information: This work was supported in part by the National Research Foundation of Korea under Grant ( NRF-2016R1A2B4014256 for S.-J.L. and Y.-S.B.; the Science Research Center NRF-2016R1A5A1009405 for S.K. and M.K.). This work was also supported by the National Institute of Supercomputing and Network/ Korea Institute of Science and Technology Information with supercomputing resources including technical support ( KSC-2015-C1-016 ). Appendix A Publisher Copyright: © 2017 Elsevier B.V.

PY - 2018/3/1

Y1 - 2018/3/1

N2 - A Zr-based metal-organic framework (MOF), UiO-66, is considered to be one of the most stable MOFs and has recently been shown to be a good candidate for adsorptive separation of Xe/Kr mixtures. Since the ability to impart chemical functionalities is an attractive characteristic of MOFs, herein, we prepared a series of functionalized UiO-66 materials (UiO-66-NH2, UiO-66-(OMe)2, UiO-66-NH2(OMe)2, and UiO-66-F4) by incorporating several polar functionalities into UiO-66. We found that series of electron-rich and electron-deficient UiO-66 materials have stronger interactions with Xe and Kr atoms than pristine UiO-66. We also found that Xe/Kr selectivity increases with the electron density of the ligand. Although there was a reduction in surface area, UiO-66-NH2(OMe)2 exhibited the highest Xe/Kr Henry's constant ratio (14.4), possibly due to having the highest electron density as well as an unsymmetrical arrangement of functional groups of the ligands. Furthermore, the breakthrough experiments show that UiO-66-NH2(OMe)2 can effectively separate Xe from Kr under dynamic mixture conditions and can be easily regenerated under a mild regeneration condition.

AB - A Zr-based metal-organic framework (MOF), UiO-66, is considered to be one of the most stable MOFs and has recently been shown to be a good candidate for adsorptive separation of Xe/Kr mixtures. Since the ability to impart chemical functionalities is an attractive characteristic of MOFs, herein, we prepared a series of functionalized UiO-66 materials (UiO-66-NH2, UiO-66-(OMe)2, UiO-66-NH2(OMe)2, and UiO-66-F4) by incorporating several polar functionalities into UiO-66. We found that series of electron-rich and electron-deficient UiO-66 materials have stronger interactions with Xe and Kr atoms than pristine UiO-66. We also found that Xe/Kr selectivity increases with the electron density of the ligand. Although there was a reduction in surface area, UiO-66-NH2(OMe)2 exhibited the highest Xe/Kr Henry's constant ratio (14.4), possibly due to having the highest electron density as well as an unsymmetrical arrangement of functional groups of the ligands. Furthermore, the breakthrough experiments show that UiO-66-NH2(OMe)2 can effectively separate Xe from Kr under dynamic mixture conditions and can be easily regenerated under a mild regeneration condition.

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JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

ER -

Adsorptive separation of xenon/krypton mixtures using ligand controls in a zirconium-based metal-organic framework

Abstract

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