A Comprehensive Cognition for the Capacity Fading Mechanism of FeS2 in
Argyrodite-based All-solid-state Lithium Battery
Abstract
Sulfide solid state electrolyte (SSE) possesses high ionic conductivity
and great processability but suffers from narrow electrochemical window.
Conversion sulfide cathode FeS2 has higher specific capacity and
moderate redox potential, making it appropriate towards sulfide SSE.
However, the complex reaction pathway and capacity fading mechanism in
FeS2 are rarely studied, especially in all-solid-state lithium battery
(ASSLB). Herein, argyrodite sulfide SSE is paired with FeS2 to
investigate the electrochemical reaction pathways and the capacity fade
mechanism. Instead of single conversion reaction, an anionic redox
driven reaction of FeS2 is revealed. The oxidization of Li2S vanishes
and large quantity of inactive Li2S accumulates to cause the interfacial
deterioration, along with the stress concentration during cycling, which
leads to the rapid capacity fade of FeS2. Finally, a simple strategy of
slurry-coated composite electrode with highly conductive network is
proposed to direct the uniform deposition of Li2S and alleviate the
stress concentration.