Abstract
The "polysulfide shuttle,"a process initiated by the dissolution of polysulfides, is recognized to be one of the major failure mechanisms of lithium-sulfur (Li-S) batteries. Much research effort has been dedicated toward efficient cathode additives and host materials to suppress the leaching of polysulfide species. Herein, we report a new 2D metal-organic framework constituted by a tritopic ligand, boron imidazolate ([BH(Im)3]-, Im = imidazole), and Co2+ ions for lithium polysulfide adsorption. The cobalt imidazolate framework (CoN6-BIF) contains octahedrally coordinated Co centers that form two-dimensional layers in the a,b plane. Composite cathodes containing CoN6-BIF exhibited high sulfur utilization and capacity retention, resulting in improved specific capacity and cycle life compared to sulfur/carbon controls. Density functional theory (DFT) calculations suggest that CoN6-BIF linkers are rotationally flexible, allowing the framework to accommodate polysulfide in the expanded pores. This unusual property of BIFs opens up new avenues for exploring flexible metal-organic frameworks (MOFs) and their applications to energy storage.
Original language | American English |
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Pages (from-to) | 10451-10458 |
Number of pages | 8 |
Journal | Chemistry of Materials |
Volume | 34 |
Issue number | 23 |
DOIs | |
State | Published - 2022 |
Bibliographical note
Publisher Copyright:© 2022 American Chemical Society.
NREL Publication Number
- NREL/JA-5900-83574
Keywords
- 2D metal-organic framework
- cathode additives
- lithium-sulfur batteries
- solar-photochemistry