A Cathode-Integrated Sulfur-Deficient Co₉S₈ Catalytic Interlayer for the Reutilization of “Lost” Polysulfides in Lithium–Sulfur Batteries

Lithium–sulfur batteries, with their high theoretical energy density and the low material cost of sulfur, are highly promising as a post-lithium ion battery contender. Their current performance is however compromised by sulfur loss and polysulfide shuttle to result in low energy efficiency and poor cycle stability. Herein, a catalytic material (Co9S8–x/CNT, nanoparticles with a metallic Co9S8 core and a sulfur-deficient shell on a CNT support) was applied as an interlayer on the sulfur cathode to retain migratory polysulfides and promote their reutilization. The Co9S8–x/CNT catalyst is highly effective for the conversion of polysulfides to insoluble end products (S or Li2S/Li2S2), and its deployment as a cathode-integrated interlayer was able to retain the polysulfides in the cathode for reuse. The accumulation of polysulfides in the electrolyte and the polysulfide shuttle were significantly reduced as a result. Consequently, a host-free sulfur cathode with the Co9S8–x/CNT interlayer had a low capacity fade rate of 0.049% per cycle for 1000 cycles at a 0.3C rate, a significant improvement of the capacity fade rate without it (0.28% per cycle for 200 cycles). The results here provide not only direct evidence for the contributions of sulfur deficiencies on the catalytic activity of Co9S8 in polysulfide conversion reactions but also the methodology on how the catalyst should be deployed in a Li–S battery for the best catalytic outcome.