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The path toward Li-ion batteries with higher energy-densities will likely involve use of thin lithium metal (Li) anode (<50 $mu$m in thickness), whose cyclability today remains limited by dendrite formation and low Coulombic efficiency. Previous studies have shown that the solid-electrolyte-interface (SEI) of Li metal plays a crucial role in Li electrodeposition and stripping. However, design rules for optimal SEIs on lithium metal are not well-established. Here, using integrated experimental and modeling studies on a series of structurally-similar SEI-modifying compounds as model systems, we reveal the relationship between SEI compositions, Li deposition morphology and coulombic efficiency, and identify two key descriptors (ionicity and compactness) for high performance SEIs through integrated experimental and modeling studies. Using this understanding, we design a highly ionic and compact SEI that shows excellent cycling performance in LiCoO$_2$-Li full cells at practical current densities. Our results provide guidance for the rational selection and optimization of SEI modifiers to further improve Li metal anodes.
Silicon is a promising candidate for negative electrodes due to its high theoretical specific capacity (~3579 mAh g-1) and low lithiation potential (~0.40 V vs Li). However, its practical applications in battery have been inhibited by the large volum
Lithium metal cells are key towards achieving high specific energy and energy density for electrification of transportation and aviation. Anode-free cells are the limiting case of lithium metal cells involving no excess lithium and the highest possib
A porous electrode resulting from unregulated Li growth is the major cause of the low Coulombic efficiency and potential safety hazards of rechargeable Li metal batteries. Strategies aiming to achieve large granular Li deposits have been extensively
A new class of high-performance pyrrolidinium cation based ionanofluid electrolytes with higher lithium salt concentration are developed. The electrolytes are formed by dispersing imidazolium ionic liquid functionalized TiO2 nanoparticles in low cond
The penetration of dendrites in ceramic lithium conductors severely constrains the development of solid-state batteries (SSBs) while its nanoscopic origin remain unelucidated. We develop an in-situ nanoscale electrochemical characterization technique