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Diversity-oriented synthesis of polymer membranes with ion solvation cages
Nature ( IF 42.778 ) Pub Date : 2021-04-07 , DOI: 10.1038/s41586-021-03377-7
Miranda J. Baran, Mark E. Carrington, Swagat Sahu, Artem Baskin, Junhua Song, Michael A. Baird, Kee Sung Han, Karl T. Mueller, Simon J. Teat, Stephen M. Meckler, Chengyin Fu, David Prendergast, Brett A. Helms

Microporous polymers feature shape-persistent free volume elements (FVEs), which are permeated by small molecules and ions when used as membranes for chemical separations, water purification, fuel cells and batteries1,2,3. Identifying FVEs that have analyte specificity remains a challenge, owing to difficulties in generating polymers with sufficient diversity to enable screening of their properties. Here we describe a diversity-oriented synthetic strategy for microporous polymer membranes to identify candidates featuring FVEs that serve as solvation cages for lithium ions (Li+). This strategy includes diversification of bis(catechol) monomers by Mannich reactions to introduce Li+-coordinating functionality within FVEs, topology-enforcing polymerizations for networking FVEs into different pore architectures, and several on-polymer reactions for diversifying pore geometries and dielectric properties. The most promising candidate membranes featuring ion solvation cages exhibited both higher ionic conductivity and higher cation transference number than control membranes, in which FVEs were aspecific, indicating that conventional bounds for membrane permeability and selectivity for ion transport can be overcome4. These advantages are associated with enhanced Li+ partitioning from the electrolyte when cages are present, higher diffusion barriers for anions within pores, and network-enforced restrictions on Li+ coordination number compared to the bulk electrolyte, which reduces the effective mass of the working ion. Such membranes show promise as anode-stabilizing interlayers in high-voltage lithium metal batteries.



中文翻译:

带有离子溶剂笼的面向多样性的聚合物膜合成

微孔聚合物具有形状持久性自由体积元素(FVE),当用作化学分离,水净化,燃料电池和电池1,2,3的膜时,会被小分子和离子渗透。由于难以产生具有足够多样性以筛选其特性的聚合物,因此鉴定具有分析物特异性的FVE仍然是一个挑战。在这里,我们描述了微孔聚合物膜的一种面向多样性的合成策略,以鉴定具有FVE的候选物,这些FVE可用作锂离子(Li +)的溶剂化笼。该策略包括通过曼尼希反应引入Li +使双(邻苯二酚)单体多样化FVE中的配位功能,将FVE连接到不同孔隙结构中的拓扑结构增强聚合,以及用于使孔隙几何形状和介电特性多样化的几种在聚合物反应。具有离子溶剂笼的最有前途的候选膜表现出比对照膜更高的离子电导率和更高的阳离子转移数,其中FVE是非特异性的,这表明可以克服膜渗透性和离子迁移选择性的常规限制4。这些优点与存在笼子时增强的Li +从电解质中的分配,更高的孔隙中阴离子的扩散壁垒以及网络对Li +的限制有关与本体电解质相比,其配位数小,从而降低了工作离子的有效质量。这种膜有望作为高压锂金属电池中稳定阳极的中间层。

更新日期:2021-04-08
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