Publication date: 10th April 2024
Transition metal fluoride (TMF) conversion-type cathodes promise up to 4 times higher gravimetric energy densities compared to common intercalation-type cathodes.
However, TMF cathodes demonstrate sluggish kinetics, poor efficiencies, and incompatibility with many liquid electrolytes. In this work, co-evaporated heterostrucutred
iron and lithium fluoride (Fe-LiF) cathodes are investigated in thin-film solid-state batteries with a LiPON electrolyte and lithium metal anode. The cells were cycled 2000
times at a cycling rate of 6C. They show a gradual improvement in voltaic efficiency (37 to 53 %) and specific capacity (146 to 216 mAh/g) during cycling. After 2000 cycles its
capacity reaches 480 mAh/g at a cycling rate of C/3.6, close to its theoretical capacity of 498 mAh/g, at room temperature conditions. This capacity gain is correlated with
an observed electrochemically activated nano-restructuring of the cathode, characterized by cycling-induced coarsening (from 2.8 to 4.2 nm) of the metallic iron phase and
its accumulation near the current collector interface, as well as lithium fluoride phase accumulation near the LiPON interface. The thin-film, solid-state setup serves as a
robust testing platform of fundamental properties of TMF conversion-type cathodes without interference from additives.
J.C. is supported by the laboratory of Thin-Films and Photovoltaics at Empa, Dubendorf. J.M. is supported by the European Union’s Horizon 2020 research and innovation programme
(grant no. 95817) and the Swiss Federal Office of Energy (SFOE, grant no. SI/502460-01). E.G is supported by Strategic Focus Area (SFA) Advanced Manufacturing, under the
”Microfluidics” project (https://www.sfa-am.ch/microfluidics.html). M.H.F. is supported by a Rubicon Fellowship from the Netherlands Organization for Scientific Research (NOW).
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