The electrochemical performance of lithium-ion batteries (LIBs) is plagued by sluggish interfacial kinetics. Fortunately, the Li solvation structure bridges the bulk electrolyte and interfacial chemistry, providing a pathway for promoting electrochemical kinetics in LIBs. Herein, we improve the interfacial kinetics by tuning the Li coordination chemistry based on solvent molecular engineering. Specifically, 4-fluorobenzyl cyanide (FBCN), featuring steric hindrance and a weak Lewis basic center, is designed to construct a bulky coordination structure with Li, weakening ion-dipole interaction (Li-solvents) but promoting coulombic attraction (Li-anions) at a normal Li salt concentration. This sterically-controlled solvation chemistry reduces the interfacial barrier and thus contributes to improved rate performance, as demonstrated practically in LiFePO//graphite pouch cells. This study provides fresh insights into solvent steric control and coordination chemistry engineering, opening a new avenue for enhancing electrochemical kinetics in LIBs.
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| http://dx.doi.org/10.1039/d4sc00013g | DOI Listing |
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