Journal
CHEM
Volume 8, Issue 7, Pages 1928-1943Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2022.03.002
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Solid-state batteries offer higher energy density and safety compared to traditional Li-ion batteries, but the usage of ceramic-based solid-state electrolytes (CSSEs) increases the interfacial resistance. This study demonstrates a breakthrough in stabilizing the LE-CSSE interface by using nanometer-scale self-assembled monolayers (SAMs), achieving unprecedented impedance approaching zero.
Solid-state batteries are highly desirable for replacing traditional Li-ion batteries to offer higher energy density and safety. However, the usage of ceramic-based solid-state electrolytes (CSSEs) leads to large interfacial resistances owing to the undesirable contact with electrodes. A small amount of organic liquid electrolyte (LE) is usually added to solve this issue. Unfortunately, a spontaneous Li+/H+ exchange reaction occurs due to the trace of proton impurity in LE accompanied by the chemical adsorption of organic decomposition, giving rise to a gradually thickened LE-CSSE interphase. Here, we demonstrate that the LE-CSSE interface can be stabilized by nanometer-scale self-assembled monolayers (SAMs) with acidic anchoring groups in which either the in situ Li+/H+ exchange or the strong interaction between CSSE and decompositions can be efficiently weakened. With the assistance of the consumption of surface Li+ concentration and the compact SAM passivating layer, unprecedented impedance approaching to zero is achieved for the active LE-CSSE interface.
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