Abstract
The advent of Li metal batteries is considered to be crucial for to ensure the ubiquity of electric transport due to their improved energy densities relative to Li-ion cells. Additionally, the electrochemical kinetics of current batteries are insufficient to provide charging times comparable to standard refueling periods, and to deliver power at reduced operating temperatures. Operating the Li metal anode under such conditions adds another layer of complexity due to the poorly understood dynamics of Li plating and stripping under kinetic stress. Though there are well-established routes to improve the kinetics associated with ion transport through the bulk electrolyte and solid-electrolyte-interphase, similar strategies for the charge-transfer barrier are limited. Our collective work aims to design the Li+ solvation structure in liquid electrolytes and to understand its impact on Li metal performance using reduced temperature operation as a tool. Specifically, we have found that the induction of ion-pairs between Li+ and anions improves such operation due to a reduction in desolvation energy understood through both experimental and advanced computational means. We have leveraged this understanding to develop electrolytes for both sulfur-type and > 4 V Li metal full batteries capable of cycling down to -60 oC. This work represents an effort to advance the understanding of electrolyte/electrode interactions from the perspective of the Li+ ion in solution.
Published Version
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