Graphene Oxide Membrane with Recognition Sites for Efficient Separation of Mono-/Di-valent Metal Ions

Xiaoyu Li, Lanying Ma, Yannan Zhou, Xiuzhen Ma, Yanfeng Cui,Haitao Feng,Wu Li,Xin Liu

Desalination（2025）

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Abstract

Extracting high-purity potassium chloride step by step from a mixed salt solution of potassium chloride and magnesium chloride after eliminating sodium chloride is a high-tech challenge. The separation of K+ and Mg2+ is quite difficult due to their similar sub-nanometer size. Herein, aniline-N-propanesulfonic acid (AnPS) with sulfonate groups was introduced to provide different ion binding affinity to improve the ion selectivity ratio of K+ and Mg2+, an ultrathin sulfonate-functionalized metal-organic framework (MOF) intercalated into a graphene oxide (GO) membrane, named GO/ZS/MOF membrane, was successfully synthesized for efficient potassium extraction. The aplenty sulfonate groups in GO sub-nanochannel membrane serve as recognition sites allowing rapid potassium ion pass through, conduciving to high potassium ion permeability. Then, the differential affinity of dehydrated K+, Li+, and Mg2+ ions to the sulfonate groups further improve the selectivity of potassium ions, the GO/ZS/MOF membrane exhibited an extraordinary selectivity of 207.7 for K+/Mg2+, 8.3 for K+/Li+ in ternary ion solution, respectively. Theoretical calculations also indicate that the difference of ion charge and binding affinity are also the main reason for the increasing of ion separation ratio except the size-sieving effect. This timely work will provide a new pathway for understanding the extraction of potassium from salt lake brine, and open up a new avenue for construction of highly permselective graphene oxide based membranes.

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Key words

Potassium extraction,Graphene oxide membrane,Ion-separation,Ternary ion solution,Transport properties,Sulfonate-functionalized metal-organic framework

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【要点】：本研究创新性地将带有磺酸基团的金属-有机框架（MOF）嵌入石墨烯氧化物（GO）膜中，制备出具有高效分离单价和双价金属离子的GO/ZS/MOF膜，实现了高纯度氯化钾的提取。

【方法】：通过引入带有磺酸基团的芳香族化合物——间苯胺丙磺酸（AnPS），提高了膜对K+和Mg2+离子的选择比，成功合成了超薄磺酸功能化的MOF/GO复合膜。

【实验】：使用GO/ZS/MOF膜在三元离子溶液中对K+和Mg2+进行分离，该膜展现出对K+/Mg2+的选择性为207.7，对K+/Li+的选择性为8.3，实验结果证明了膜对K+的高效提取能力。