Publication date: 10th April 2024
Most highly-conducting solid electrolytes decompose at the low operating potentials of next-generation anodes leading to irreversible lithium loss and increased cell resistance. Such performance losses due to electrochemical decomposition may be prevented by designing electrolytes which are thermodynamically stable at low operating potentials.
Here, we report on the discovery a new family of fully-reduced electrolytes by dissolving lithium nitride into the Li2S antifluorite structure, yielding highly conducting crystalline Li2+xS1-xNx phases, synthesized by mechanochemistry, identified by x-ray and neutron diffraction, and reaching high ionic conductivities (> 0.2 mS cm-1) at ambient temperatures. Combining impedance spectroscopy experiments and ab-initio density functional theory calculations we clarify the mechanism by which increased configurational entropy boosts ionic conductivity in Li2+xS1-xNx phases by five orders of magnitude compared to the Li2S host structure.
This advance is achieved through a novel theoretical framework, leveraging percolation analysis with local-environment-specific calculated activation barriers and is widely applicable to disordered solid electrolytes. Finally, we introduce the concept of “trapped” Li ions and how they may play an essential role when rationalizing changes in the Arrhenius prefactors from variable‑temperature conductivity measurements of disordered solid electrolytes. These findings pave the way to understanding the effect of disorder (and high-entropy) on ion-conduction in highly relevant disordered electrolyte and electrode battery materials. Additionally, we leverage the mechanistic insight developed here, to design a new class of highly-conducting solid electrolytes that could help eliminate decomposition‑induced Li losses on the anode side in high-performance next-generation batteries.
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