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Title
Morphology-controlled metal-organic frameworks as molecular traps for enhanced ion dynamics in practical semi-solid lithium metal batteries
KIAS Author
Lee, Yeongkyu
Journal
CHEMICAL ENGINEERING JOURNAL, 2024
Archive
Abstract
Controlling electrostatic interactions between charged molecules is crucial to enabling advanced batteries with reliable lithium (Li)-ion conductors. To address this issue, herein, we present a class of morphology-controlled metal-organic frameworks (MOFs) that serve as Li+ boosting molecular traps for fast Li+ conduction. A rodlike MOF is incorporated into semi-interpenetrating polymer networks to construct Li+ boosting fluidic nanochannels, which enable fast Li+ transport (sigma = 1.5 mS cm-1, tLi+ = 0.76) through the ionic pathway. Molecular dynamics simulations further elucidate the Li+ transport mechanism in these MOF-based molecular traps. This unusual Li+ conduction behavior of MOF-based semi-solid electrolytes suppresses the anion-triggered ion concentration gradient and facilitates the electrochemical reaction kinetics at the electrodes, ultimately improving the rate performance and cycling retention of Li-metal cells (consisting of LiNi0.7Co0.2Mn0.1O2 cathodes and Limetal anodes). Notably, a scalable pouch-type semi-solid Li-metal cell provides stable cycling performance for realistic batteries, exceeding those of previously reported Li batteries including porous crystalline frameworks.