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A multiwalled carbon nanotube/sulfur (MWCNT@S) composite with core-shell structure was successfully embedded into the interlay galleries of graphene sheets (GS) through a facile two-step assembly process. Scanning and transmission electron microscopy images reveal a 3D hierarchical sandwich-type architecture of the composite GS-MWCNT@S. The thickness of the S layer on the MWCNTs is ~20 nm. Raman spectroscopy, X-ray diffraction, thermogravimetric analysis, and energy-dispersive X-ray analysis confirm that the sulfur in the composite is highly crystalline with a mass loading up to 70% of the composite. This composite is evaluated as a cathode material for Li/S batteries. The GS-MWCNT@S composite exhibits a high initial capacity of 1396 mAh/g at a current density of 0.2C (1C = 1672 mA/g), corresponding to 83% usage of the sulfur active material. Much improved cycling stability and rate capability are achieved for the GS-MWCNT@S composite cathode compared with the composite lacking GS or MWCNT. The superior electrochemical performance of the GS-MWCNT@S composite is mainly attributed to the synergistic effects of GS and MWCNTs, which provide a 3D conductive network for electron transfer, open channels for ion diffusion, strong confinement of soluble polysulfides, and effective buffer for volume expansion of the S cathode during discharge.

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Cathode materials with high energy density, long cycle life, and low cost are of top priority for energy storage systems. The Li‐rich transition metal (TM) oxides achieve high specific capacities by redox reactions of both the TM and oxygen ions. However, the poor reversible redox reaction of the anions results in severe fading of the cycling performance. Herein, the vacancy‐containing Na4/7[Mn6/7(◻Mn)1/7]O2 (◻Mn for vacancies in the MnO slab) is presented as a novel cathode material for Na‐ion batteries. The presence of native vacancies endows this material with attractive properties including high structural flexibility and stability upon Na‐ion extraction and insertion and high reversibility of oxygen redox reaction. Synchrotron X‐ray absorption near edge structure and X‐ray photoelectron spectroscopy studies demonstrate that the charge compensation is dominated by the oxygen redox reaction and Mn3+/Mn4+ redox reaction separately. In situ synchrotron X‐ray diffraction exhibits its zero‐strain feature during the cycling. Density functional theory calculations further deepen the understanding of the charge compensation by oxygen and manganese redox reactions and the immobility of the Mn ions in the material. These findings provide new ideas on searching for and designing materials with high capacity and high structural stability for novel energy storage systems.

The development of safe, stable, and long-life Li-ion batteries is being intensively pursued to enable the electrification of transportation and intelligent grid applications. Here, we report a new solid-state Li-ion battery technology, using a solid nanocomposite electrolyte composed of porous silica matrices with in situ immobilizing Li(+)-conducting ionic liquid, anode material of MCMB, and cathode material of LiCoO2, LiNi1/3Co1/3Mn1/3O2, or LiFePO4. An injection printing method is used for the electrode/electrolyte preparation. Solid nanocomposite electrolytes exhibit superior performance to the conventional organic electrolytes with regard to safety and cycle-life. They also have a transparent glassy structure with high ionic conductivity and good mechanical strength. Solid-state full cells tested with the various cathodes exhibited high specific capacities, long cycling stability, and excellent high temperature performance. This solid-state battery technology will provide new avenues for the rational engineering of advanced Li-ion batteries and other electrochemical devices.