Robust metal-organic framework monoliths for long-term cycling lithium metal batteries
JOURNAL OF MATERIALS CHEMISTRY A(2024)
摘要
Lithium metal with low electrochemical potential and high theoretical capacity has attracted significant attention as an anode material for high-energy-density batteries. However, the practical application of Li metal anodes has been inhibited by the growth of Li dendrites during charge-discharge cycling. Nano- or micro-porous layers have been introduced at the Li/electrolyte interface to regulate the Li+ flux and stabilize the Li metal anode. However, such interlayers fabricated via slurry-casting have non-uniform porous structures containing interparticle voids due to the binders and solvents, which reduces the efficacy of the interlayer in suppressing dendritic Li growth. Herein, we report mechanically robust void-free metal-organic framework (MOF) monoliths that can effectively homogenize the Li+ flux and suppress dendritic growth. MOF monoliths (500 nm-thick) are directly grown on a polypropylene separator without binders via a simple chemical route with a void-free structure and mechanical robustness (Young's modulus of similar to 7.8 GPa). The monolithic MOF film facilitates the filtration of large anions through the nanopores, resulting in an increased Li+ transference number. Furthermore, electrochemical simulations and experiments confirm that MOF monoliths with well-ordered nanopores but without interparticle voids effectively redistribute the locally concentrated Li+ flux over the Li anode, leading to reversible Li plating and stripping. A Li metal battery (full cell) with MOF monoliths operates stably over 300 cycles with a capacity retention of 96.6%. The interlayer design proposed in this study offers the possibility of commercializing high-energy-density Li metal batteries with long cycle lifetimes. A monolithic MOF layer is synthesized on a porous separator via a simple chemical route, which effectively homogenizes the Li+ flux through its nanopores and physically blocks the growth of Li dendrites.
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