Optimized Adsorption–Catalytic Conversion for Lithium Polysulfides by Constructing Bimetallic Compounds for Lithium–Sulfur Batteries

Although lithium–sulfur batteries possess the advantage of high theoretical specific capacity, the inevitable shuttle effect of lithium polysulfides is still a difficult problem restricting its application. The design of highly active catalysts to promote the redox reaction during charge–discharge and thus reduce the existence time of lithium polysulfides in the electrolyte is the mainstream solution at present. In particular, bimetallic compounds can provide more active sites and exhibit better catalytic properties than single-component metal compounds by regulating the electronic structure of the catalysts. In this work, bimetallic compounds-nitrogen-doped carbon nanotubes (NiCo)Se2-NCNT and (CuCo)Se2-NCNT are designed by introducing Ni and Cu into CoSe2, respectively. The (CuCo)Se2-NCNT delivers an optimized adsorption–catalytic conversion for lithium polysulfide, benefitting from adjusted electron structure with downshifted d-band center and increased electron fill number of Co in (CuCo)Se2 compared with that of (NiCo)Se2. This endows (CuCo)Se2 moderate adsorption strength for lithium polysulfides and better catalytic properties for their conversion. As a result, the lithium–sulfur batteries with (CuCo)Se2-NCNT achieve a high specific capacity of 1051.06 mAh g−1 at 1C and an enhanced rate property with a specific capacity of 838.27 mAh g−1 at 4C. The work provides meaningful insights into the design of bimetallic compounds as catalysts for lithium–sulfur batteries.