MOFs derived ZnSe/N-doped carbon nanosheets as multifunctional interlayers for ultralong-Life lithium-sulfur batteries

doi:10.1016/j.jmst.2022.02.030

Abstract

Abstract:

The shuttle effect and slow conversion rate of lithium polysulfides (LiPSs) have become the main obstructs to the development of lithium-sulfur (Li-S) batteries. Herein, the low cost metal-organic frameworks derived nitrogen-doped carbon nanosheets embedded with zinc selenide nanoparticles (ZnSe/NC nanosheets) were designed and synthesized for Li-S batteries. As the LiPSs trapping-layer, these nanocomposites provide some key benefits: (1) The nitrogen doping changes local electron distribution in the carbon nanosheets, thus the electrical conductivity is greatly improved for facilitating the transport of electrons/ions. (2) Nitrogen atoms and ZnSe nanoparticles play an important role in anchoring the LiPSs via chemical interactions. (3) The remarkable catalytic activity of ZnSe nanoparticles can accelerate the redox kinetics of LiPSs. As a result, the Li-S battery with the ZnSe/NC nanosheets modified separator exhibits ultralong lifespan over 1500 cycles with a small capacity loss of only 0.046% per cycle at 1 C, which is superior over those reported values. Furthermore, the Li-S battery with a high sulfur loading of 4.71 mg cm^-2 can still maintain a high areal capacity of 4.28 mAh cm^-2 after 50 cycles. This work provides a new route to the design of multifunctional low cost and high-performance separators for remarkably stable Li-S batteries.

Key words: Lithium-sulfur batteries, Metal-organic frameworks, Zinc selenide, Multifunctional separator, Adsorption and catalysis

Biao Wang, Dongyue Sun, Yilun Ren, Xiaoya Zhou, Yujie Ma, Shaochun Tang, Xiangkang Meng. MOFs derived ZnSe/N-doped carbon nanosheets as multifunctional interlayers for ultralong-Life lithium-sulfur batteries[J]. J. Mater. Sci. Technol., 2022, 125: 97-104.

Figures/Tables 6

Fig. 1. Schematic illustration of (a) the synthesis process of ZnSe/NC nanosheets, and (b) a Li-S battery with the ZnSe/NC nanosheets as a multifunctional interlayer.

Fig. 2. TEM images of (a, d) Zn-MOF, (b, e) NC nanosheets, and (c, f, g) ZnSe/NC nanosheets; (h) Fourier-transformed crystalline lattice form (g); (i) SAED patterns of ZnSe/NC nanosheets.

Fig. 3. (a) XRD patterns, (b) Raman spectrum, and (c) N2 sorption isotherm of NC and ZnSe/NC nanosheets; XPS spectra of ZnSe/NC nanosheets-(d) Survey spectrum, (e-h) high-resolution XPS of C 1s, N 1s, Zn 2p, and Se 3d, respectively; SEM images of ZnSe/NC-separator-(i) Top-view, (j) cross-section; (k) digital photos of ZnSe/NC-separator.

Fig. 4. (a) CV curves at a scan rate of 0.3 mV s-1; (b) values of peak voltages obtained from the CV curves; (c) EIS of different cells before cycling; CV curves of cells with (d) ZnSe/NC-separator, (e) NC-separator, and (f) KB-separator at different scan rates; plot of CV peak current versus square root scan rates for the cells with (g) ZnSe/NC-separator, (h) NC-separator, and (i) KB-separator.

Fig. 5. (a) Rate capacity of different cells; GCD profiles of (b) different cells at 0.1 C, (c) ZnSe/NC-separator cell at different current densities, and (d) ZnSe/NC-separator cell at different cycles at 0.2 C; GITT voltage profiles of cells with (e) ZnSe/NC-separator, (f) NC-separator, and (g) KB-separator at 0.1 C; (h) prolonged cycling performance of ZnSe/NC-separator cell at 1 C; (i) cell performance comparison with previously reported Li-S cells.

Fig. 6. (a) Digital image of Li2S6 solutions containing blank, KB, NC, and ZnSe/NC; (b) UV-Vis spectra of the Li2S6 solution mixed with the different adsorbents after 6 h; high resolution XPS spectra of (c) N 1s and (d) Zn 2p for ZnSe/NC before and after adsorption of Li2S6; (e) cycling performance at 5 C; (f) cycling performance at 0.1 C with different S loadings.

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