Single-atom-layer traps in a solid electrolyte for lithium batteries

Abstract

In order to fully understand the lithium-ion transport mechanism in solid electrolytes for batteries, not only the periodic lattice but also the non-periodic features that disrupt the ideal periodicity must be comprehensively studied. At present only a limited number of nonperiodic features such as point defects and grain boundaries are considered in mechanistic studies. Here, we discover an additional type of non-periodic feature that significantly influences ionic transport; this feature is termed a "single-atom-layer trap" (SALT). In a prototype solid electrolyte Li 0.33 La 0.56 TiO 3 , the single-atom-layer defects that form closed loops, i.e., SALTs, are found ubiquitous by atomic-resolution electron microscopy. According to ab initio calculations, these defect loops prevent large volumes of materials from participating in ionic transport, and thus severely degrade the total conductivity. This discovery points out the urgency of thoroughly investigating different types of non-periodic features, and motivates similar studies for other solid electrolytes.

Atomistic Insights into the Effects of Doping and Vacancy Clustering on Li-Ion Conduction in the Li3OCl Antiperovskite Solid Electrolyte

“…Solid electrolytes have attracted significant research in recent years due to the safety, stability, and energy density benefits, which solid-state batteries can provide over conventional liquid electrolyte systems. − In particular, solid electrolytes may enable the use of high-voltage electrodes or lithium–metal anodes, which are incompatible with current liquid electrolytes. − , However, despite the potential benefits of solid electrolytes, transport issues at the electrode interface and the reduced ionic conductivity versus their liquid counterparts have thus far prevented their widespread adoption. ,,,, …”

Dendrites in Solid‐State Batteries: Ion Transport Behavior, Advanced Characterization, and Interface Regulation

“…first reported a novel defect called “single‐atom‐layer trap” using TEM, which was a nucleation point of the dendrite (Figure 12h). [ 153 ] Furthermore, the functional interface observed by high‐resolution STEM confirms a facile Li‐transport, and offers possibilities for dendrite‐free metal anode. Due to the contact between Li 7−3 x Al x La 3 Zr 2 O 12 (LLZO) and Li metal anode, Ma et al.…”

“…In addition to grain boundaries, pores, and cracks that have been widely reported, there are also 2D defects in typical Li 0.33 La 0.56 TiO 3 (LLTO) planes called as “single‐atom‐layer trap”. The defect is first discovered and can critically influence ionic migration, [ 153 ] which is conducive to gain an in‐depth understanding of the ion transport mechanism.…”

“…Reproduced with permission. [ 153 ] Copyright 2017, American Chemical Society. i) 5 units interphase formation at the lithium|LLZO.…”

Synthesis Strategies, Catalytic Applications, and Performance Regulation of Single‐Atom Catalysts

“…batteries. [ 147–153 ] Among them, Li–S batteries (LSBs) with high theoretical energy capacity of 1675 mA h g −1 and abundant resources of S on earth are recognized as one of the most promising choices for advanced energy storage. However, their practical applications are facing pressing challenges such as shuttling of polysulfide, poor electrical conductivity of active S and formed Li 2 S that insoluble damaging to lithium polysulfides (LiPSs) redox.…”