Hierarchically 3D structured milled lamellar MoS2/nano-silicon@carbon hybrid with medium capacity and long cycling sustainability as anodes for lithium-ion batteries

doi:10.1016/j.jmst.2019.05.002

Abstract

Abstract:

A hierarchically 3D structured milled lamellar MoS₂/nano-silicon@carbon hybrid with medium capacity and long-term lifespan is designed by a green and scalable approach using ball milling process and spray-drying/pyrolysis routes. The microspheres consist of low-content nano-silicon (20 wt%), milled lamellar MoS₂ sheets and porous carbon skeletons. A mixture of silicon nanoparticles and MoS₂ flakes serves as an inner core, while porous carbon pyrolyzed from petroleum pitch acts as a protective shell. The particular architecture affords robust mechanical support, abundant buffering space and enhanced electrical conductivity, thus effectively accommodating drastic volume variation during repetitive Li⁺ intercalation/extraction. The Si/MoS₂@C hybrid delivers a high initial discharge specific capacity of 1257.8 mA h g^-1 and exhibits a reversible capacity of 767.52 mA h g^-1 at a current density 100 mA g^-1 after 250 cycles. Most impressively, the electrode depicts a superior long-cycling durability with a discharge capacity of 537.6 mA h g^-1 even after 1200 cycles at a current density of 500 mA g^-1. Meanwhile, the hybrid also shows excellent rate performance such as 388.1 mA h g^-1 even at a large current density of 3000 mA g^-1.

Key words: Si, MoS₂, Medium capacity, Long-term lifespan, Lithium ion batteries

Zhang Peng, Ru Qiang, Yan Honglin, Hou Xianhua, Chen Fuming, Hu Shejun, Zhao Lingzhi. Hierarchically 3D structured milled lamellar MoS₂/nano-silicon@carbon hybrid with medium capacity and long cycling sustainability as anodes for lithium-ion batteries[J]. J. Mater. Sci. Technol., 2019, 35(9): 1840-1850.

Figures/Tables 13

Scheme 1. Schematic illustration of milled lamellar MoS2/nano-silicon@carbon.

Fig. 1. (a) XRD pattern and (b) Raman spectra of SMC, (c) optical image of SMP precursor and final product SMC.

Fig. 2. SEM images of (a-d) SMC microsphere.

Fig. 3. (a-c) TEM images, (d-f) HRTEM images, (g) Nitrogen absorption-desorption isotherms and (h) BJH pore size distribution.

Fig. 4. CV profiles of (a) Nano-silicon, (b) Commercial MoS2 and (c) SMC in the initial 3 cycles at a scan rate of 0.2 mV/s, (d) Galvanostatic charge-discharge curves of SMC for the 1 st, 2nd and 250th cycles at a current density of 100 mA g-1.

Fig. 5. Comparable cycling performance of various SMP (7:3, 8:2 and 1:1) precursors and final product SMC hybrid at a constant current density of 100 and 500 mA g-1.

Fig. 6. (a) Rate performance of final product SMC at various current densities from 100 to 3000 mA g-1, (b) Cycling performance of Si, MoS2, SMP precursor and final product SMC at a constant current density of 100 mA g-1, (c) Super long service life of final product SMC at a constant current density of 500 mA g-1.

Fig. 7. (a-b) SEM, (c-d) TEM images and (e-h) EDS mapping of final product SMC electrode after 1200 cycles at a current density of 500 mA g-1 (the blue, red, purple and green dots stand for Si, C, Mo and S, respectively).

Fig. 8. The simulated geometry structures of (a) bulk MoS2, (b) bulk Si, (c) Si/C interface, (d) MoS2/C interface.

Fig. 9. Band structures of (a) bulk MoS2, (b) bulk Si, (c) MoS2 (002)/C (002) interface, (d) Si (111)/C (002) interface.

Fig. 10. Work functions of (a) MoS2 (002) plane, (b) Si (111) plane, (c) C (002) plane, (d) MoS2 (002)/C (002) and (e) Si (111)/C (002) interface.

Fig. 11. Partial density of states of (a) Mo, (b) S and (c) C atoms and (d) Total density of states of MoS2 (002)/C (002) interface.

Fig. 12. Partial density of states of (d) Si, (e) C atoms and (f) Total density of states of MoS2 (002)/C (002) interface.

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Hierarchically 3D structured milled lamellar MoS₂/nano-silicon@carbon hybrid with medium capacity and long cycling sustainability as anodes for lithium-ion batteries

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