A series of solid solutions (Li 2 Fe 1−y Mn y )SO with a cubic antiperovskite structure was successfully synthesized. The composition (Li 2 Fe 0.5 Mn 0.5 )SO was intensively studied as a cathode in Li-ion batteries showing a reversible specific capacity of 120 mA h g −1 and almost a 100% Coulombic efficiency after 50 cycles at 0.1C meaning extraction/insertion of 1 Li per formula unit during 10 h. Operando X-ray absorption spectroscopy confirmed the redox activity of both Fe 2+ and Mn 2+ cations during battery charge and discharge, while operando synchrotron X-ray diffraction studies revealed a reversible formation of a second isostructural phase upon Li-removal and insertion at least for the first several cycles. In comparison to (Li 2 Fe)SO, the presence of Mn stabilizes the crystal structure of (Li 2 Fe 0.5 Mn 0.5 )SO during battery operation, although post mortem TEM studies confirmed a gradual amorphization after 50 cycles. A lower specific capacity of (Li 2 Fe 0.5 Mn 0.5 )SO in comparison to (Li 2 Fe)SO is probably caused by slower kinetics, especially in the two-phase region, as confirmed by Li-diffusion coefficient measurements.

A tunable redox potential and electrochemical performance are realized by anionic substitution of S by Se for the Li-rich antiperovskite (Li2Fe)SO cathode.

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Solid solutions of 2D transition metal trihalides are rapidly growing in interest for the search for new 2D materials with novel properties at nanoscale dimensions. In this regard, we present...

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