Anomalous High Ionic Conductivity of Nanoporous β-Li₃PS₄

Abstract

Lithium-ion-conducting solid electrolytes hold promise for enabling high-energy battery chemistries and circumventing safety issues of conventional lithium batteries. Achieving the combination of high ionic conductivity and a broad electrochemical window in solid electrolytes is a grand challenge for the synthesis of battery materials. Herein we show an enhancement of the room-temperature lithium-ion conductivity by 3 orders of magnitude through the creation of nanostructured Li(3)PS(4). This material has a wide electrochemical window (5 V) and superior chemical stability against lithium metal. The nanoporous structure of Li(3)PS(4) reconciles two vital effects that enhance the ionic conductivity: (1) the reduction of the dimensions to a nanometer-sized framework stabilizes the high-conduction β phase that occurs at elevated temperatures, and (2) the high surface-to-bulk ratio of nanoporous β-Li(3)PS(4) promotes surface conduction. Manipulating the ionic conductivity of solid electrolytes has far-reaching implications for materials design and synthesis in a broad range of applications, including batteries, fuel cells, sensors, photovoltaic systems, and so forth.

Structural limitations for optimizing garnet-type solid electrolytes: a perspective

“…such as Li 3 PS 4 and Li 10 SnP 2 S 14 ) available, where targeted structural chemistry might lead to the desired properties. 4,[77][78][79][80][81][82][83][84] …”

Effect of the binder content on the electrochemical performance of composite cathode using Li6PS5Cl precursor solution in an all-solid-state lithium battery

“…In the preparation of Li PS Cl through the solution process, ethanol was used for the solvent [ 6 ]. Other solvents used to prepare solid electrolyte solutions are anhydrous hydrazine [ 7 ] (Li Ge P S , σ = 1.82 × 10 S/cm), tetrahydrofuran [ 8 ] (β Li PS , σ = 1.6 × 10 S/cm), acetonitrile [ 9 ] (Li P S I, σ = 6.3 × 10 S/cm), methylformamide [ 10 ] (Li PS , σ = 2.6 × 10 S/cm), methanol [ 11 ] (LiI Li SnS , σ = 4.1 × 10 S/cm), and ethanol [ 6 ] (Li PS Cl, σ = 1.4 × 10 S/cm). Solvents such as methanol or ethanol are more attractive to scalable procedures since they have low boiling points that allow the composite cathode to be obtained easily.…”

Modeling interfaces between solids: Application to Li battery materials

“…In addition, we also consider Li 2 O/Li interfaces which have been studied by a number of authors. [14][15][16][17][18][19][20][21][22] While these interfaces are predominantly related to possible electrolyte/anode materials in Li ion batteries, 23 our methodology should apply equally well to solid state cathode interfaces. 11,24 The manuscript is organized as follows.…”