Oxidized Nb2C MXene as catalysts for lithium-sulfur batteries: Mitigating the shuttle phenomenon by facilitating catalytic conversion of lithium polysulfides

doi:10.1016/j.jmst.2021.10.025

Abstract

Abstract:

Extensive research has been devoted to lithium-sulfur (Li-S) batteries due to their overwhelming promises and advantages such as high theoretical capacity (1675 mAh g^-1), extremely cost effectiveness and abundance and availability of sulfur. Nevertheless, a sluggish electrochemical kinetics of the battery limited by a slow conversion of lithium polysulfide (LiPSs) intermediates and LiPSs shuttle effect severely hinder its development towards industrial application. Herein, we designed the oxidized Nb₂C MXene with amorphous carbon (Nb₂O₅/C) composites as sulfur host using CO₂ treatment to address the above issues. The Nb₂O₅/C composites with high conductivity are directly employed as sulfur hosts for Li-S battery capable to remarkably mitigate the shuttle phenomenon due to a combined effect of their LiPSs trapping ability and catalytic activity towards their accelerated conversion. Meanwhile, the unique layered structure of the composite facilitates ion transfer and accommodates the volume changes of the cathode during cycling. With this rational design, the resultant Li-S batteries exhibit superior electrochemical performance with a high initial specific capacity of 745 mAh g^-1 at 1.0 C and a reversible capacity of 620 mAh g^-1 at a high rate cycling at 3.0 C.

Key words: Oxidized Nb₂C Mxene, Li-S batteries, Lithium polysulfides conversion, Electrochemical performance

Cailing Song, Wen Zhang, Qianwen Jin, Yan Zhao, Yongguang Zhang, Xin Wang, Zhumabay Bakenov. Oxidized Nb₂C MXene as catalysts for lithium-sulfur batteries: Mitigating the shuttle phenomenon by facilitating catalytic conversion of lithium polysulfides[J]. J. Mater. Sci. Technol., 2022, 119: 45-52.

Figures/Tables 7

Scheme 1. Schematic of the synthesis of S/Nb2O5/C.

Fig. 1. SEM images of (a) Nb2C, (b) Nb2O5/C and (c) corresponding elemental mapping of Nb2O5/C. (d) TEM image of Nb2O5/C. (e) HRTEM image and (f) corresponding its FFT, inverse FFT, and lattice spacing images of Nb2O5/C. (g) High-magnification elemental mapping of Nb2O5/C.

Fig. 2. (a) XRD patterns, (b) Raman spectra, (c) Nb 3d, (d) O 1s XPS spectra, (e) nitrogen adsorption/desorption isotherms of the Nb2O5/C and Nb2O5. (f) TGA profiles of the S/Nb2O5/C and S/Nb2O5.

Fig. 3. (a) Schematic illustration of LiPSs conversion on Nb2O5/C. (b) Photographs and UV-vis spectra of Li2S6 solution adsorbed by Nb2O5 and Nb2O5/C. (c) S 2p high-resolution XPS spectra of pristine Li2S6 and Li2S6 adsorbed by Nb2O5/C. (d) The Gibbs free energy profiles of LiPSs on Nb2O5/C and Nb2O5. (e) Binding energies of LiPSs on Nb2O5/C and Nb2O5. Calculated density of states of (f) Nb2O5 and (g) Nb2O5/C.

Fig. 4. (a) CV curves at 6 mV s-1 of Nb2O5/C and Nb2O5 symmetric cells. (b) The first three CV curves of Nb2O5/C symmetric cell at 6 mV s-1. (c) The EIS plots of Nb2O5/C and Nb2O5 symmetric cells. Li2S deposition profiles of (d) Nb2O5/C and (e) Nb2O5. (f) The LSV curves of Li2S oxidization for Nb2O5 and Nb2O5/C.

Fig. 5. (a) CV curves of S/Nb2O5/C electrode at 0.1 mV s-1. (b) The voltage profile of S/Nb2O5/C and (c) cycling performance of S/Nb2O5/C and S/Nb2O5 electrodes at 0.2 C. (d) The rate performances of S/Nb2O5/C and S/Nb2O5 electrodes and (e) voltage profile of S/Nb2O5/C electrodes from 0.2 C to 3.0 C. (f) The EIS plots of S/Nb2O5/C and S/Nb2O5 electrodes. (g) Long cyclic performances of S/Nb2O5/C and S/Nb2O5 electrodes at 1.0 C for 300 cycles. (h) Cycle performance at 0.1 C of S/Nb2O5/C under raised sulfur loading and limited electrolyte.

Fig. 6. CV curves at various scan rates for (a) S/Nb2O5/C and (b) S/Nb2O5. Linear matching of peak point currents for (c) S/Nb2O5/C and (d) S/Nb2O5.

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Oxidized Nb₂C MXene as catalysts for lithium-sulfur batteries: Mitigating the shuttle phenomenon by facilitating catalytic conversion of lithium polysulfides

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