Cation-selective two-dimensional polyimine membranes for high-performance osmotic energy conversion

Zhen Zhang; Preeti Bhauriyal; Hafeesudeen Sahabudeen; Zhiyong Wang; Xiaohui Liu; Mike Hambsch; Stefan C.B. Mannsfeld; Renhao Dong; Thomas Heine; Xinliang Feng

doi:10.1038/s41467-022-31523-w

Cation-selective two-dimensional polyimine membranes for high-performance osmotic energy conversion

Zhen Zhang, Preeti Bhauriyal, Hafeesudeen Sahabudeen, Zhiyong Wang, Xiaohui Liu, Mike Hambsch, Stefan C.B. Mannsfeld, Renhao Dong, Thomas Heine, Xinliang Feng

Department of Chemistry

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

19 Citations (Scopus)

Abstract

Two-dimensional (2D) membranes are emerging candidates for osmotic energy conversion. However, the trade-off between ion selectivity and conductivity remains the key bottleneck. Here we demonstrate a fully crystalline imine-based 2D polymer (2DPI) membrane capable of combining excellent ionic conductivity and high selectivity for osmotic energy conversion. The 2DPI can preferentially transport cations with Na⁺ selectivity coefficient of 0.98 (Na⁺/Cl⁻ selectivity ratio ~84) and K⁺ selectivity coefficient of 0.93 (K⁺/Cl⁻ ratio ~29). Moreover, the nanometer-scale thickness (~70 nm) generates a substantially high ionic flux, contributing to a record power density of up to ~53 W m⁻², which is superior to most of nanoporous 2D membranes (0.8~35 W m⁻²). Density functional theory unveils that the oxygen and imine nitrogen can both function as the active sites depending on the ionization state of hydroxyl groups, and the enhanced interaction of Na⁺ versus K⁺ with 2DPI plays a significant role in directing the ion selectivity.

Original language	English
Article number	3935
Journal	Nature communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-022-31523-w
Publication status	Published - 2022 Dec

Bibliographical note

Funding Information:
This work was financially supported by the European Union’s Horizon 2020 research and innovation programme under grant agreement No 881603, the European Science Foundation (ESF), and the Coordination Networks: Building Blocks for Functional Systems (SPP1928, COORNET), CRC1415, ERC Grants on T2DCP and FC2DMOF (No. 852909). We acknowledge Elettra Sincrotrone Trieste for providing access to its synchrotron radiation facilities and we thank Luisa Barba for assistance in using beamline XRD1. The research leading to this result has been supported by the project CALIPSOplus under Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. Z.Z. acknowledges the support of the Alexander von Humboldt Foundation.

Publisher Copyright:
© 2022, The Author(s).

All Science Journal Classification (ASJC) codes

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
General
Physics and Astronomy(all)

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title = "Cation-selective two-dimensional polyimine membranes for high-performance osmotic energy conversion",

abstract = "Two-dimensional (2D) membranes are emerging candidates for osmotic energy conversion. However, the trade-off between ion selectivity and conductivity remains the key bottleneck. Here we demonstrate a fully crystalline imine-based 2D polymer (2DPI) membrane capable of combining excellent ionic conductivity and high selectivity for osmotic energy conversion. The 2DPI can preferentially transport cations with Na+ selectivity coefficient of 0.98 (Na+/Cl− selectivity ratio ~84) and K+ selectivity coefficient of 0.93 (K+/Cl− ratio ~29). Moreover, the nanometer-scale thickness (~70 nm) generates a substantially high ionic flux, contributing to a record power density of up to ~53 W m−2, which is superior to most of nanoporous 2D membranes (0.8~35 W m−2). Density functional theory unveils that the oxygen and imine nitrogen can both function as the active sites depending on the ionization state of hydroxyl groups, and the enhanced interaction of Na+ versus K+ with 2DPI plays a significant role in directing the ion selectivity.",

author = "Zhen Zhang and Preeti Bhauriyal and Hafeesudeen Sahabudeen and Zhiyong Wang and Xiaohui Liu and Mike Hambsch and Mannsfeld, {Stefan C.B.} and Renhao Dong and Thomas Heine and Xinliang Feng",

note = "Funding Information: This work was financially supported by the European Union{\textquoteright}s Horizon 2020 research and innovation programme under grant agreement No 881603, the European Science Foundation (ESF), and the Coordination Networks: Building Blocks for Functional Systems (SPP1928, COORNET), CRC1415, ERC Grants on T2DCP and FC2DMOF (No. 852909). We acknowledge Elettra Sincrotrone Trieste for providing access to its synchrotron radiation facilities and we thank Luisa Barba for assistance in using beamline XRD1. The research leading to this result has been supported by the project CALIPSOplus under Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. Z.Z. acknowledges the support of the Alexander von Humboldt Foundation. Publisher Copyright: {\textcopyright} 2022, The Author(s).",

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AU - Bhauriyal, Preeti

AU - Sahabudeen, Hafeesudeen

AU - Wang, Zhiyong

AU - Liu, Xiaohui

AU - Hambsch, Mike

AU - Mannsfeld, Stefan C.B.

AU - Dong, Renhao

AU - Heine, Thomas

AU - Feng, Xinliang

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PY - 2022/12

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N2 - Two-dimensional (2D) membranes are emerging candidates for osmotic energy conversion. However, the trade-off between ion selectivity and conductivity remains the key bottleneck. Here we demonstrate a fully crystalline imine-based 2D polymer (2DPI) membrane capable of combining excellent ionic conductivity and high selectivity for osmotic energy conversion. The 2DPI can preferentially transport cations with Na+ selectivity coefficient of 0.98 (Na+/Cl− selectivity ratio ~84) and K+ selectivity coefficient of 0.93 (K+/Cl− ratio ~29). Moreover, the nanometer-scale thickness (~70 nm) generates a substantially high ionic flux, contributing to a record power density of up to ~53 W m−2, which is superior to most of nanoporous 2D membranes (0.8~35 W m−2). Density functional theory unveils that the oxygen and imine nitrogen can both function as the active sites depending on the ionization state of hydroxyl groups, and the enhanced interaction of Na+ versus K+ with 2DPI plays a significant role in directing the ion selectivity.

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Cation-selective two-dimensional polyimine membranes for high-performance osmotic energy conversion

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