Journal
ADVANCED MATERIALS
Volume 34, Issue 23, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202201410
Keywords
covalent organic frameworks; flexible electrolytes; foldable batteries; lithium-metal batteries; solid-state batteries
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Funding
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering [DE-SC0005397]
- KAUST Competitive Fund [URF/1/3769-01]
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This study presents a solid-state electrolyte based on covalent organic framework (COF) that exhibits high Li+ conductivity and enhanced mechanical toughness. By solidifying a tailored liquid electrolyte in situ, the charge-carrier concentration in the COF channels is increased, resulting in a 100-fold increase in Li+ conductivity. The COF membrane also demonstrates foldable solid-state pouch cell capabilities.
Solid-state electrolytes with high Li+ conductivity, flexibility, durability, and stability offer an attractive solution to enhance safety and energy density. However, meeting these stringent requirements poses challenges to the existing solid polymeric or ceramic electrolytes. Here, an electrolyte-mediated single-Li+-conductive covalent organic framework (COF) is presented, which represents a new category of quality solid-state Li+ conductors. In situ solidification of a tailored liquid electrolyte boosts the charge-carrier concentration in the COF channels, decouples Li+ cations from both COF walls and molecular chains, and eliminates defects by crystal soldering. Such an altered microenvironment activates the motion of Li+ ions in a directional manner, which leads to an increase in Li+ conductivity by 100 times with a transference number of 0.85 achieved at room temperature. Moreover, the electrolyte conversion cements the ultrathin COF membrane with fortified mechanical toughness. With the COF membrane, foldable solid-state pouch cells are demonstrated.
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