Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation

Eunji Choi; Ji Il Choi; Yong Jae Kim; Yeong Jae Kim; Kiwon Eum; Yunkyu Choi; Ohchan Kwon; Minsu Kim; Wooyoung Choi; Hyungjoon Ji; Seung Soon Jang; Dae Woo Kim

doi:10.1002/anie.202214269

Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation

Eunji Choi, Ji Il Choi, Yong Jae Kim, Yeong Jae Kim, Kiwon Eum, Yunkyu Choi, Ohchan Kwon, Minsu Kim, Wooyoung Choi, Hyungjoon Ji, Seung Soon Jang, Dae Woo Kim

Department of Chemical and Biomolecular Engineering

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

Abstract

Zeolitic imidazolate frameworks (ZIFs) are promising for gas separation membrane, but their molecular cut-off differs from that expected from its intrinsic aperture structure because of their flexibility. Herein, we introduced graphene nanoribbons (GNRs) to rigidify the ZIF framework. Because the sp² edge of the GNRs induces strong anchoring effects, the modified layer can be rigidified. Particularly, when the GNRs were embedded and distributed in the ZIF-8 layer, an intrinsic aperture size of 3.4 Å was observed, resulting in high H₂/CO₂ separation (H₂ permeance: 5.2×10⁻⁶ mol/m² Pa s, ideal selectivity: 142). The performance surpasses the upper bound of polycrystalline MOF membrane performance. In addition, the membrane can be applied to blue H₂ production, as demonstrated with a simulated steam reformed gas containing H₂/CO₂/CH₄. The separation performance was retained in the presence of water. The fundamentals of the molecular transport through the rigid ZIF-8 framework were revealed using molecular dynamics simulations.

Original language	English
Article number	e202214269
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	49
DOIs	https://doi.org/10.1002/anie.202214269
Publication status	Published - 2022 Dec 5

Bibliographical note

Funding Information:
This study was supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (NRF‐2020R1C1C1003289), and by the Technology Innovation Program (20013621, Center for Super Critical Material Industrial Technology), funded by the Ministry of Trade, Industry and Energy (MOTIE, Korea).

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)

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10.1002/anie.202214269

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title = "Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation",

abstract = "Zeolitic imidazolate frameworks (ZIFs) are promising for gas separation membrane, but their molecular cut-off differs from that expected from its intrinsic aperture structure because of their flexibility. Herein, we introduced graphene nanoribbons (GNRs) to rigidify the ZIF framework. Because the sp2 edge of the GNRs induces strong anchoring effects, the modified layer can be rigidified. Particularly, when the GNRs were embedded and distributed in the ZIF-8 layer, an intrinsic aperture size of 3.4 {\AA} was observed, resulting in high H2/CO2 separation (H2 permeance: 5.2×10−6 mol/m2 Pa s, ideal selectivity: 142). The performance surpasses the upper bound of polycrystalline MOF membrane performance. In addition, the membrane can be applied to blue H2 production, as demonstrated with a simulated steam reformed gas containing H2/CO2/CH4. The separation performance was retained in the presence of water. The fundamentals of the molecular transport through the rigid ZIF-8 framework were revealed using molecular dynamics simulations.",

author = "Eunji Choi and Choi, {Ji Il} and Kim, {Yong Jae} and Kim, {Yeong Jae} and Kiwon Eum and Yunkyu Choi and Ohchan Kwon and Minsu Kim and Wooyoung Choi and Hyungjoon Ji and Jang, {Seung Soon} and Kim, {Dae Woo}",

note = "Funding Information: This study was supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (NRF‐2020R1C1C1003289), and by the Technology Innovation Program (20013621, Center for Super Critical Material Industrial Technology), funded by the Ministry of Trade, Industry and Energy (MOTIE, Korea). Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH.",

year = "2022",

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doi = "10.1002/anie.202214269",

language = "English",

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T1 - Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation

AU - Choi, Eunji

AU - Choi, Ji Il

AU - Kim, Yong Jae

AU - Kim, Yeong Jae

AU - Eum, Kiwon

AU - Choi, Yunkyu

AU - Kwon, Ohchan

AU - Kim, Minsu

AU - Choi, Wooyoung

AU - Ji, Hyungjoon

AU - Jang, Seung Soon

AU - Kim, Dae Woo

N1 - Funding Information: This study was supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (NRF‐2020R1C1C1003289), and by the Technology Innovation Program (20013621, Center for Super Critical Material Industrial Technology), funded by the Ministry of Trade, Industry and Energy (MOTIE, Korea). Publisher Copyright: © 2022 Wiley-VCH GmbH.

PY - 2022/12/5

Y1 - 2022/12/5

N2 - Zeolitic imidazolate frameworks (ZIFs) are promising for gas separation membrane, but their molecular cut-off differs from that expected from its intrinsic aperture structure because of their flexibility. Herein, we introduced graphene nanoribbons (GNRs) to rigidify the ZIF framework. Because the sp2 edge of the GNRs induces strong anchoring effects, the modified layer can be rigidified. Particularly, when the GNRs were embedded and distributed in the ZIF-8 layer, an intrinsic aperture size of 3.4 Å was observed, resulting in high H2/CO2 separation (H2 permeance: 5.2×10−6 mol/m2 Pa s, ideal selectivity: 142). The performance surpasses the upper bound of polycrystalline MOF membrane performance. In addition, the membrane can be applied to blue H2 production, as demonstrated with a simulated steam reformed gas containing H2/CO2/CH4. The separation performance was retained in the presence of water. The fundamentals of the molecular transport through the rigid ZIF-8 framework were revealed using molecular dynamics simulations.

AB - Zeolitic imidazolate frameworks (ZIFs) are promising for gas separation membrane, but their molecular cut-off differs from that expected from its intrinsic aperture structure because of their flexibility. Herein, we introduced graphene nanoribbons (GNRs) to rigidify the ZIF framework. Because the sp2 edge of the GNRs induces strong anchoring effects, the modified layer can be rigidified. Particularly, when the GNRs were embedded and distributed in the ZIF-8 layer, an intrinsic aperture size of 3.4 Å was observed, resulting in high H2/CO2 separation (H2 permeance: 5.2×10−6 mol/m2 Pa s, ideal selectivity: 142). The performance surpasses the upper bound of polycrystalline MOF membrane performance. In addition, the membrane can be applied to blue H2 production, as demonstrated with a simulated steam reformed gas containing H2/CO2/CH4. The separation performance was retained in the presence of water. The fundamentals of the molecular transport through the rigid ZIF-8 framework were revealed using molecular dynamics simulations.

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Graphene Nanoribbon Hybridization of Zeolitic Imidazolate Framework Membranes for Intrinsic Molecular Separation

Abstract

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