Electrochemical-repaired porous graphene membranes for precise ion-ion separation

Zongyao Zhou, Kangning Zhao, Heng-Yu Chi, Yueqing Shen, Shuqing Song, Kuang-Jung Hsu, Mojtaba Chevalier, Wenxiong Shi and Kumar Varoon Agrawal ()
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Zongyao Zhou: École Polytechnique Fédérale de Lausanne (EPFL)
Kangning Zhao: École Polytechnique Fédérale de Lausanne (EPFL)
Heng-Yu Chi: École Polytechnique Fédérale de Lausanne (EPFL)
Yueqing Shen: École Polytechnique Fédérale de Lausanne (EPFL)
Shuqing Song: École Polytechnique Fédérale de Lausanne (EPFL)
Kuang-Jung Hsu: École Polytechnique Fédérale de Lausanne (EPFL)
Mojtaba Chevalier: École Polytechnique Fédérale de Lausanne (EPFL)
Wenxiong Shi: Tianjin University of Technology
Kumar Varoon Agrawal: École Polytechnique Fédérale de Lausanne (EPFL)

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract The preparation of atom-thick porous lattice hosting Å-scale pores is attractive to achieve a large ion-ion selectivity in combination with a large ion flux. Graphene film is an ideal selective layer for this if high-precision pores can be incorporated, however, it is challenging to avoid larger non-selective pores at the tail-end of the pore size distribution which reduces ion-ion selectivity. Herein, we develop a strategy to overcome this challenge using an electrochemical repair strategy that successfully masks larger pores in large-area graphene. 10-nm-thick electropolymerized conjugated microporous polymer (CMP) layer is successfully deposited on graphene, thanks to a strong π-π interaction in these two materials. While the CMP layer itself is not selective, it effectively masks graphene pores, leading to a large Li+/Mg2+ selectivity from zero-dimensional pores reaching 300 with a high Li+ ion permeation rate surpassing the performance of reported materials for ion-ion separation. Overall, this scalable repair strategy enables the fabrication of monolayer graphene membranes with customizable pore sizes, limiting the contribution of nonselective pores, and offering graphene membranes a versatile platform for a broad spectrum of challenging separations.

Date: 2024
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DOI: 10.1038/s41467-024-48419-6

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