Constructing Co/CoV2O6 tandem catalytic heterostructure to enhance lithium polysulfide conversion in lithium-sulfur batteries

ABSTRACT The “shuttle effect” caused by polysulfide (LiPSs) dissolution and diffusion is a great challenge for sulfur (S) cathode in lithium-sulfur batteries (LSBs). Herein, we have successfully constructed Co/CoV 2 O 6 tandem catalytic heterostructure anchored by N-doped carbon (Co/CoV 2 O 6 /NC) via an impregnation-assisted pyriaolysis method. The “adsorption-transfer-conversion” tandem catalytic mechanism for LiPSs is realized by utilizing the three behaviors of the strong chemical adsorption of CoV 2 O 6 to LiPSs, the strong conversion of Co to LiPSs, and the transport effect of CoV 2 O 6 ←Co interfacial built-in electric field to polysulfide ions. This can effectively suppress the “shuttle effect” by separating the adsorption and conversion process of LiPSs at different active sites. The tandem catalytic characteristic coupled with the interfacial Co-N and V-N bonds among Co, CoV 2 O 6 and NC, the high electrical conductivities of metal Co and NC conducting network, the hierarchical porous structure of polyhedral framework, collectively endow Co/CoV 2 O 6 /NC@S cathode with strong structural stability, weak electrochemical polarization, good electrochemical reversibility and fast electrochemical kinetics. As a result, Co/CoV 2 O 6 /NC@S cathode presents the significantly enhanced electrochemical performance with a high capacity of 558.4 mAh g -1 at 0.2   C after 100 cycles and a low-capacity decay rate of 0.123% per cycle during 300 cycles at 1   C.