| Summary: | <p>Nitrogenous solid electrolytes such as lithium phosphorus oxynitride (LiPON) have effectual interfacial compatibility with lithium metal; in part, this has enabled the development of thin-film solid-state batteries with excellent long-term cycling performance. However, most known nitrogen-containing solid electrolytes lack the ionic conductivity required for high-power/high-capacity batteries; therefore, the development of new nitrogenous solid electrolytes with increased ionic conductivity is highly desirable. The mechanical milling of lithium nitride (Li<sub>3</sub>N) with phosphorus pentasulfide (P<sub>2</sub>S<sub>5</sub>) has previously been reported to produce amorphous lithium-ion conductors, but the composition of these materials and the reactions occurring during the milling processes were hitherto undetermined. Here, we show that mechanochemically milled Li<sub>3</sub>N·P<sub>2</sub>S<sub>5</sub> solid electrolytes contain less nitrogen than expected as N<sub>2</sub> gas is released during an early stage of the ball milling process. Li<sub>3</sub>N·P<sub>2</sub>S<sub>5</sub> solid electrolytes are mixtures composed of multiple lithium thiophosphates, lithium sulfide, and red phosphorus. We show that amorphous Li<sub>3</sub>PS<sub>4</sub> is responsible for the ionic conductivity of Li<sub>3</sub>N·P<sub>2</sub>S<sub>5</sub> electrolytes produced by ball milling.</p>
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