Modulating charge transport in MOFs with zirconium oxide nodes and redox-active linkers for lithium sulfur batteries
- Resource Type
- Authors
- V. Sara Thoi; Avery E. Baumann; Bingqian Liu
- Source
- Polyhedron. 170:788-795
- Subject
- 010405 organic chemistry
Chemistry
Oxide
chemistry.chemical_element
010402 general chemistry
Electrochemistry
01 natural sciences
Redox
Sulfur
Energy storage
0104 chemical sciences
Inorganic Chemistry
Metal
chemistry.chemical_compound
Chemical engineering
visual_art
Materials Chemistry
visual_art.visual_art_medium
Physical and Theoretical Chemistry
Dissolution
Polysulfide
- Language
- ISSN
- 0277-5387
Despite the promises of high specific energy density and low cost, lithium sulfur (Li-S) batteries still face major challenges in long-term cyclability due to polysulfide dissolution. Metal–organic frameworks (MOFs) have unique advantages as porous sulfur hosts due to their high chemical and structural tunability. Herein, we demonstrate that MOFs consisting of functionalized metal oxide nodes and redox-active linkers influence charge transport and enhance Li-S cycling. We show that anthraquinone-based Zr-MOF composite cathodes display higher maximum capacity and longer cycle life compared to sulfur/carbon electrodes. Lithiating the terminal ligands and bridging hydroxides in the Zr6(μ3-O)4(μ3-OH)4 nodes further improves battery performance at high charge rates. We hypothesize that the additional redox sites within the linkers and the presence of lithiated clusters permit greater electrochemical accessibility to the polysulfides by providing additional electron and ion conduction pathways. Moreover, the pore structure plays a critical role in available conduction pathways. Our efforts demonstrate the utility of metal oxide clusters for modulating charge transport and provide structure–function relationships to direct design of novel materials for energy storage devices.