Diversity-oriented synthesis of polymer membranes with ion solvation cages

微型多孔材料 溶剂化 电解质 聚合物 化学工程 离子 离子键合 分子 材料科学 化学 纳米技术 有机化学 物理化学 工程类 生物化学 电极
作者
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
出处
期刊:Nature [Nature Portfolio]
卷期号:592 (7853): 225-231 被引量:127
标识
DOI:10.1038/s41586-021-03377-7
摘要

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 batteries1-3. 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.
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