Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving

Abstract Two-dimensional (2D) metal-organic framework (MOF) nanosheet membranes hold promise for exact molecular transfer due to their structural diversity and well-defined in-plane nanochannels. However, achieving precise regulation of stacking modes between neighboring nanosheets in membrane appli...

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Main Authors: Wufeng Wu, Xitai Cai, Xianfeng Yang, Yanying Wei, Li Ding, Libo Li, Haihui Wang
Format: Article
Language:English
Published: Nature Portfolio 2024-12-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-54663-7
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author Wufeng Wu
Xitai Cai
Xianfeng Yang
Yanying Wei
Li Ding
Libo Li
Haihui Wang
author_facet Wufeng Wu
Xitai Cai
Xianfeng Yang
Yanying Wei
Li Ding
Libo Li
Haihui Wang
author_sort Wufeng Wu
collection DOAJ
description Abstract Two-dimensional (2D) metal-organic framework (MOF) nanosheet membranes hold promise for exact molecular transfer due to their structural diversity and well-defined in-plane nanochannels. However, achieving precise regulation of stacking modes between neighboring nanosheets in membrane applications and understanding its influence on separation performance remains unrevealed and challenging. Here, we propose a strategy for accurately controlling the stacking modes of MOF nanosheets via linker polarity regulation. Both theoretical calculations and experimental results demonstrate that a high linker polarity promotes neighboring nanosheets to a maximum AB stacking due to steric hindrance effects, leading to a controlled effective pore size of the membrane and consequently to improved molecular sieving. Among series of CuBDC-based 2D MOFs with different linkers, the CuBDC-NO2 nanosheet membranes exhibit a reduced effective stacking aperture of 0.372 nm, yielding H2 permeance of 4.44 × 10−7 mol m−2 s−1 Pa−1 with a high H2/CO2 and H2/CH4 selectivity of 266 and 536, respectively. This work represents the in-depth investigation of the accurate tuning of MOF nanosheet stacking in the field of 2D materials, offering more perspectives for broader applications with universality for various 2D materials.
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publishDate 2024-12-01
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spelling doaj-art-f7c0094881f24d1f946c236602cb9d132025-01-05T12:35:08ZengNature PortfolioNature Communications2041-17232024-12-011511910.1038/s41467-024-54663-7Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sievingWufeng Wu0Xitai Cai1Xianfeng Yang2Yanying Wei3Li Ding4Libo Li5Haihui Wang6State Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of TechnologyState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of TechnologyAnalytical and Testing Centre, South China University of TechnologyState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of TechnologyBeijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua UniversityState Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of TechnologyBeijing Key Laboratory for Membrane Materials and Engineering, Department of Chemical Engineering, Tsinghua UniversityAbstract Two-dimensional (2D) metal-organic framework (MOF) nanosheet membranes hold promise for exact molecular transfer due to their structural diversity and well-defined in-plane nanochannels. However, achieving precise regulation of stacking modes between neighboring nanosheets in membrane applications and understanding its influence on separation performance remains unrevealed and challenging. Here, we propose a strategy for accurately controlling the stacking modes of MOF nanosheets via linker polarity regulation. Both theoretical calculations and experimental results demonstrate that a high linker polarity promotes neighboring nanosheets to a maximum AB stacking due to steric hindrance effects, leading to a controlled effective pore size of the membrane and consequently to improved molecular sieving. Among series of CuBDC-based 2D MOFs with different linkers, the CuBDC-NO2 nanosheet membranes exhibit a reduced effective stacking aperture of 0.372 nm, yielding H2 permeance of 4.44 × 10−7 mol m−2 s−1 Pa−1 with a high H2/CO2 and H2/CH4 selectivity of 266 and 536, respectively. This work represents the in-depth investigation of the accurate tuning of MOF nanosheet stacking in the field of 2D materials, offering more perspectives for broader applications with universality for various 2D materials.https://doi.org/10.1038/s41467-024-54663-7
spellingShingle Wufeng Wu
Xitai Cai
Xianfeng Yang
Yanying Wei
Li Ding
Libo Li
Haihui Wang
Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
Nature Communications
title Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
title_full Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
title_fullStr Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
title_full_unstemmed Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
title_short Accurate stacking engineering of MOF nanosheets as membranes for precise H2 sieving
title_sort accurate stacking engineering of mof nanosheets as membranes for precise h2 sieving
url https://doi.org/10.1038/s41467-024-54663-7
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AT xianfengyang accuratestackingengineeringofmofnanosheetsasmembranesforpreciseh2sieving
AT yanyingwei accuratestackingengineeringofmofnanosheetsasmembranesforpreciseh2sieving
AT liding accuratestackingengineeringofmofnanosheetsasmembranesforpreciseh2sieving
AT liboli accuratestackingengineeringofmofnanosheetsasmembranesforpreciseh2sieving
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