Lithium complexing strategy based on host-guest recognition for efficient Mg2+/Li+ separation

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2025-01-05 DOI:10.1016/j.watres.2025.123100

Xiangmin Xu , Xiaowei Zhu , Jinchao Chen , Xingran Zhang , Zhiwei Wang , Fang Li

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Abstract

Ion selective membranes with precise Mg²⁺/Li⁺ separation have attracted extensive interest in lithium extraction to circumvent the lithium supply shortage. However, realizing this target remains a significant challenge mainly due to a high concentration ratio of Mg²⁺/Li⁺ as well as the relatively close ionic hydration radius and chemical. Herein, inspired by the host-guest recognition between alkali-metal ions and crown ether (CE), a novel approach was proposed to regulate the membrane internal structure by introducing CE to strengthen the complexation between Li⁺ and CE. The CE modified membranes achieved the unique outcome of “Li⁺ rejection-Mg²⁺ permeation” deriving from enhanced solubility (K_S) and retarded diffusivity (D_S) of Li⁺ compared to that of Mg²⁺. The Mg²⁺/Li⁺ separation factors for MgSO₄/Li₂SO₄ and MgCl₂/LiCl of modified membranes (i.e., 20.1 and 17.7) are about 21.9 and 19.9 time higher than that of pristine membranes, respectively. The results from density function theory (DFT) indicated that the stronger host-guest interaction between CE and Li⁺ combined them closely, thereby increasing solubility and reducing diffusivity of Li⁺. Our findings develop a new efficient membrane-based strategy enabling the production of high-purity lithium salts from simulated brine.

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基于主客体识别的锂络合策略对Mg2+/Li+的高效分离

具有精确Mg2+/Li+分离的离子选择膜在锂提取方面引起了广泛的兴趣，以避免锂供应短缺。然而，实现这一目标仍然是一个重大的挑战，主要是由于Mg2+/Li+的高浓度比以及相对接近的离子水合半径和化学性质。本文受碱金属离子与冠醚（CE）之间主客体识别的启发，提出了一种通过引入CE加强Li+与CE之间的络合来调节膜内部结构的新方法。与Mg2+相比，CE修饰膜的Li+溶解度（KS）提高，扩散率（DS）减慢，从而实现了“Li+排斥-Mg2+渗透”的独特效果。改性膜对MgSO4/Li2SO4和MgCl2/LiCl的Mg2+/Li+分离因子（分别为20.1和17.7）分别比未改性膜高21.9倍和19.9倍。密度泛函理论（DFT）结果表明，CE与Li+之间较强的主客体相互作用使它们紧密结合，从而增加了Li+的溶解度，降低了Li+的扩散系数。我们的发现开发了一种新的高效的基于膜的策略，可以从模拟盐水中生产高纯度的锂盐。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.

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