Lithium Batteries: Unraveling the Intra and Intercycle Interfacial Evolution of Li₆PS₅Cl‐Based All‐Solid‐State Lithium Batteries (Adv. Energy Mater. 4/2020)

Abstract

In article number 1903311, Wenkui Zhang and co‐workers perform in situ and ex situ measurements to monitor the interfacial evolutions in an all‐solid‐state LiNi0.8Co0.1Mn0.1O2/Li6PS5Cl/Li battery. The interfacial evolutions (changes of space charge layer and chemical bond vibration) are very different inter‐ and intracycle. Li+ ion migration has a significant influence on these interfacial behaviors.

In Situ Deprotection of Polymeric Binders for Solution‐Processible Sulfide‐Based All‐Solid‐State Batteries

“…[ 22 ] The distinct cyclability of the (deprotect) TBA‐ b ‐BR cell was reflected in its CEs. As recognized commonly for sulfide‐based ASSBs, [ 23 ] all three of the cells adversely experienced relatively low initial CEs (76.3, 73.3, and 67.8%, respectively) due to the known thermodynamically unstable nature of LPSCl at high voltages, [ 21 ] which lead to the formation of a passivation layer on the SE. Nevertheless, the CE of the (deprotect) TBA‐ b ‐BR cell increased more rapidly from the 2nd cycle compared to those of the other two cells (Figure S11d, Supporting Information).…”

Interfacial Reactions in Inorganic All‐Solid‐State Lithium Batteries

“…In Figure 5f, the in‐situ Raman spectroscopy measurements to monitor the detailed interface evolutions in NMC811/Li 6 PS 5 Cl/Li cell. While the interface reaction occurs, the Li + migration can also cause a slight change of PS 4 3− structure at interface [105a] . In addition to these interface evolutions, interfacial reactions also cause the chemo‐mechanical failure at interface [105c,107] .…”

“…[106], copyright 2019, American Chemical Society. f) Schematic illustrations of interface evolutions during the charge‐discharge processes based on different vibration states of P−S bond in PS 4 3− at NCM/Li 6 PS 5 Cl interface [105a] . Reproduced with permission from Ref.…”

“…To be more specific, the cathode/SSE interface is suffering from undesirable element diffusion and side reactions due to the narrow electrochemical window of SSEs, [16a] the interface instability result in increasing interfacial impedance and deteriorating battery performance. For the lithium/SE interface, since the strong reductive lithium, almost all the typically SSEs (such as Li 7 P 3 S 11 , [16a] Li 3 PS 4 , [135] argyrodite [105a] ) are suffering from chemically unstable issues after contact with lithium metal, thus giving rise to the growth of Li dendrites along the SSEs, and the resulting decomposition products have low ionic conductivity and high electronic conductivity [136] . To alleviate these serious interface problems of SSEs, many efforts have been carried out.…”

Designing Ceramic/Polymer Composite as Highly Ionic Conductive Solid‐State Electrolytes

“…The chemical reaction at the interface between electrolytes and cathode is complicated. Even the contact between two different ceramic lithium‐ion conductors can lead to resistance [122,123] . Although C/PCEs can block the contact between the ceramic modifier and the active material of cathode, the poor thermal stability, and low oxidation potential of the polymer still limit the improvement effect of C/PCEs on the positive electrode interface.…”