Argyrodite Solid Electrolyte-Integrated Ni-Rich Oxide Cathode with Enhanced Interfacial Compatibility for All-Solid-State Lithium Batteries

Abstract

All-solid-state lithium batteries (ASSLBs) paired with an argyrodite sulfide solid electrolyte have become a candidate to take the world by storm for achieving high energy and safety. However, the undesirable interface design between a sulfide solid electrolyte and cathode is difficult to address its scalability production challenge. Particularly, the inferior interfacial contact between a sulfide solid electrolyte and cathode is an intractable obstacle for the large-scale commercial application of ASSLBs. Herein, an elaborately designed conformally in situ integration of a sulfide solid electrolyte onto a Ni-rich oxide cathode is proposed to overcome this issue through a facile tape casting method. In this unique integrated electrode structure, the sulfide solid electrolyte intimately makes contact with the Ni-rich oxide cathode, which significantly strengthens the solid–solid interfacial compatibility, as well as decreases the interfacial reaction resistances, thereby enabling rapid Li+ transportation and a stable interfacial structure. As a result, ASSLBs consisting of a sulfide solid electrolyte-integrated Ni-rich oxide cathode and Li anode exhibit high discharge capacity, excellent cyclic stability, and remarkable rate performance, which are superior to the cells with segregated structures composed of a Ni-rich oxide cathode, sulfide solid electrolyte, and Li anode. The features clearly indicate that the advanced interfacial contact between the cathode and solid electrolyte is responsible for ASSLBs with low polarization and fast reaction kinetics. Therefore, this work provides a rational proof-of-concept fabrication protocol for the reliable interfacial structure design of high-performance ASSLBs.

Charge fluctuation drives anion rotation to enhance the conductivity of Na11M2PS12 (M = Si, Ge, Sn) superionic conductors

“…This journal is © the Owner Societies 2023 semiconducting materials usually increases with temperature; therefore, the conductivity trend of the material should follow the same order. However, our observation for these materials shows Na11 Si 2 PS 12 4 Na 11 Ge 2 PS 12 4 Na 11 Sn 2 PS 12 at high temperature and Na 11 Si 2 PS 12 o Na 11 Ge 2 PS 12 o Na 11 Sn 2 PS 12 at low temperature. To figure out the fundamental reason for this phenomenon, we performed the following analysis.…”

“…[2][3][4][5][6][7] Among them, lithium-ion batteries have been widely studied for their outstanding merits, such as high energy densities and long calendar lives. [8][9][10][11] However, being a rare metal, the feasibility of lithium's large-scale applications has become a serious concern. Sodium-ion batteries gradually attracted attention and can potentially be the alternative to lithium-ion batteries with good safety and offer the advantage of a natural abundance of sodium resources.…”

Halogen‐Rich Lithium Argyrodite Solid‐State Electrolytes: A Review

“…Xia et al [82] . designed a novel integrated electrode structure by coating the LPSC‐1.5‐ x NBR electrolyte slurry onto the surface of the obtained dried NCM811 cathode (Figure 6a).…”

“…Xia et al [82] designed a novel integrated electrode structure by coating the LPSC-1.5-xNBR electrolyte slurry onto the surface of the obtained dried NCM811 cathode (Figure 6a). Toluene and butyl butyrate were chosen as solvents because of their compatibility with argyrodite electrolytes.…”

Microbe‐Mediated Biosynthesis of Multidimensional Carbon‐Based Materials for Energy Storage Applications

“…Lithium-sulfur (Li-S) batteries with high theoretical capacity (1675 mAh g −1 ), high energy density (2567 Wh kg −1 ), environmental friendliness, and abundant resource of sulfur are widely applied in electronic devices and aerospace fields, etc. [214][215][216] However, several scientific and technological issues of sulfur-based cathodes impede the commercial application of Li-S batteries, including: [217][218][219] 1) Poor electron/ion conductivity of active sulfur and the produced lithium sulfide, resulting in low electrochemical reaction kinetics. 2) The high-volume expansion (80%) during the conversion process of sulfur to lithium sulfide, leading to the destruction and pulverization of the structure.…”