Catalytic polysulfides immobilization within a S/C-Co-N hollow cathode obtained by nonthermal imprison route

Abstract

Lithium-sulfur (Li-S) batteries have hitherto attracted dramatic research interests as an optional high-energy output candidate to replace the traditional lithium-ion batteries on account of its high energy density and low cost. Nonetheless, their kinetics arrearage and detrimental "shuttling effect" caused by the migration of soluble lithium polysulfide (LiPS) intermediates severely limit its practical application. Here, by a nonthermal route sulfur is in-situ imprisoned into Co/N-codoped hollow carbon sphere (NC-Co) to construct an integrated S/C-Co-N hollow cathode (S@NC-Co) and directly applied in Li-S batteries, which effectively avoids complex template removal and sulfur infiltration process. The hollow NC-Co sphere not only restricts polysulfides migration via physical confinement but also enhances polysulfides conversion through redox-active electro-catalysis. Moreover, the hollow structure has large cavity offering sufficient space to accommodate volume expansion and excellent conductivity promising efficient electron/charge transfer. As a result, the batteries assembled by the S@NC-Co cathode achieve low polarization and high-rate capability (551 mAh g^-1 at 4C). Remarkably, the batteries also present an outstanding long-term durability over 800 cycles at 1C, in which the capacity attenuation is merely 0.06 % per cycle. This work demonstrates a novel strategy in designing hierarchical structures or nanoreactors for electrochemical reactions and energy storage systems.

Keywords: Catalytic conversion; Hollow structure; Nonthermal route; Polysulfides immobilization; Sulfur cathode.