Corresponding Author

Pei-Kang Shen(pkshen@gxu.edu.cn)


Lithium-sulfur (Li-S) batteries are considered as a promising energy storage device due to their ultrahigh theoretical energy density of 2500 Wh·kg-1 and low cost. However, the practical application of Li-S batteries is seriously limited by their low actual energy density, the shuttle effect of polysulfides (LiPSs), and the insulating nature of sulfur and lithium sulfides. Carbon materials have been developed in the design of sulfur hosts due to their adjustable pore structure and high electrical conductivity, but their non-polar surfaces have weak interactions with LiPSs. Herein, MXene-carbon black/sulfur (Ti3C2Tx-CB/S) composites were prepared and applied to the integrated electrodes of Li-S batteries. The CB/S was prepared via a melting-diffusion method and Ti3C2Tx MXene nanosheets were synthesized by etching Ti3AlC2 MAX with LiF/HCl. After mixing CB/S and Ti3C2Tx , Ti3C2Tx-CB/S cathode material was obtained and coated on commercial separator (PP) to prepare Ti3C2Tx-CB/S-PP integrated electrodes. On the one hand, the two-dimensional Ti3C2Tx nanosheets dispersed in the CB/S particles not only serve as multiple physical barriers to inhibit the diffusion of LiPSs, but also have strong chemical interactions with them, effectively alleviating the shuttle effect. Thus, Ti3C2Tx improves the conductivity of CB/S composite, which is beneficial to the reaction kinetics of the cathode. Furthermore, the design of Ti3C2Tx-CB/S-PP integrated electrode increases the energy density of Li-S batteries. X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) were employed to analyze the structures, morphologies, and surface chemical composition of the synthesized materials. The results of constant current charge/discharge tests showed that Ti3C2Tx-CB/S-PP electrode achieved superior rate performance and cycling performance than CB/S-PP electrode. The initial discharge capacity of Ti3C2Tx-CB/S-PP electrode at 0.1 C current was 1028.8 mAh·g-1, higher than 896.8 mAh·g-1 of CB/S-PP electrode. The cycling test at 0.2 C indicated that Ti3C2Tx-CB/S-PP maintained a discharge capacity of 726.4 mAh·g-1 after 80 cycles, better than CB/S-PP (529.2 mAh·g-1). Moreover, due to the improved utilization of the active material at the interface between the cathode and the separator, Ti3C2Tx-CB/S-PP electrode also showed better cycling stability compared to the Ti3C2Tx-CB/S-Al electrode based on the traditional aluminum foil current collector. The capacity degradation rate of Ti3C2Tx-CB/S-PP was only 0.072% per cycle in a long-term cycling test of 400 cycles at 0.5 C, while that of Ti3C2Tx-CB/S-Al was 0.10%. The strategy of using Ti3C2Tx-CB/S to construct an integrated electrode provides a new direction for Li-S batteries with high performance and high energy density.

Graphical Abstract


lithium-sulfur batteries, integrated electrode, shuttle effect, Ti3C2Tx MXene

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