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Halide Heterogeneous Structure Boosting Ionic Diffusion and High-voltage Stability of Sodium Superionic Conductors

May 10, 2024

Given the growing scarcity of lithium resources, solid-state sodium-ion batteries (SSSBs) have garnered significant attention owing to their sustainable composition, high theoretical energy density, and inherent safety advantages. The development of SSSBs heavily hinges on the development of a superionic Na+ conductor (SSC) that features high conductivity, (electro)chemical stability, and deformability. The construction of heterogeneous structures offers a promising approach to comprehensively enhancing these properties in a way that differs from traditional structural optimization. This work exploits the structural variance between high and low-coordination halide frameworks to develop a new class of halide heterogeneous structure electrolytes (HSEs). The halide HSEs incorporating a UCl3-type high-coordination framework and amorphous low-coordination phase achieves the highest known Na+ conductivity among halide SSCs. By discerning the individual contribution of the crystalline bulk, amorphous region, and interface, this work unravels the synergistic ion conduction within halide HSEs and provides a comprehensive explanation of the amorphization effect. More importantly, the excellent deformability, high-voltage stability, and expandability of HSEs enable effective SSSB integration.

Authors

Yifei Mo (University of Maryland)

Additional Materials

U.S. National Science Foundation and NSF DMREF, Materials for Our Future

This material is based upon work supported by the U.S. National Science Foundation Award No. 2015237. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the U.S. National Science Foundation. This site is maintained collaboratively by principal investigators with NSF DMREF awards, independent of the NSF.