Mechanistic Insights on the Mesoscale in the Positive Electrode of Lithium–Sulfur Batteries

• A comprehensive description of the electrochemical processes in the positive electrodeof lithium–sulfur batteries is critical to the enhancement of sulfur utilization. However,the discharge mechanisms are complicated due to the various reactions in multiplephases and the tortuosity of the highly porous carbon matrix. While previous studieshave focused on the precipitation of Li2S, the effect of the limited mass transport insidethe micro-/mesopores of an electrode with optimized surface area have largely beenneglected. In this work, operando small-angle scattering with three different contrasts,and wide-angle scattering, has been performed with simultaneous resistance measure-ment of internal and diffusion. The results indicate that both electrode passivation andcomplete pore blockage are unlikely since the precipitates are surrounded by the elec-trolyte and grow mostly in number, not in size. The difference between the small- andwide-angle scattering reveals the amorphous discharge products at a low C-rate. Furtheranalyses demonstrate the correlation between the diffusion resistance and the contrastin the mesopores at the end of discharge, which suggests that Li-ion deficiency is thelimiting factor of sulfur utilization at a medium C-rate.

Ämnesord

NATURVETENSKAP  -- Kemi -- Oorganisk kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)

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