How to exert the energy density advantage is a key link in the development of lithium–sulfur batteries. Therefore, the performance degradation of high-sulfur-loading cathodes becomes an urgent problem to be solved at present. In addition, the volumetric capacities of high-sulfur-loading cathodes are still at a low level compared with their areal capacities. Aiming at these issues, two-dimensional carbon yolk-shell nanosheet is developed herein to construct a novel self-supporting sulfur cathode. The cathode with high-sulfur loading of 5 mg cm−2 and sulfur content of 73 wt% not only delivers an excellent rate performance and cycling stability, but also provides a favorable balance between the areal (5.7 mAh cm–2) and volumetric (1330 mAh cm–3) capacities. Remarkably, an areal capacity of 11.4 mAh cm–2 can be further achieved by increasing the sulfur loading from 5 to 10 mg cm–2. This work provides a promising direction for high-energy-density lithium–sulfur batteries.
Graphene
nanoscroll (GNS) is a spirally wrapped two-dimensional
(2D) graphene sheet (GS) with a 1D tubular structure resembling that
of a multiwalled carbon nanotube (MWCNT). GNS provide open structure
at both ends and interlayer galleries that can be easily intercalated
and adjusted, which show great potential applications in energy storage.
Here we demonstrate a novel and simple strategy for the large-scale
preparation of GNSs wrapping Fe3O4 nanoparticles
(denoted as Fe3O4@GNSs) from graphene oxide
(GO) sheets by cold quenching in liquid nitrogen. When a heated aqueous
mixed suspension of GO sheets and Fe3O4 nanoparticles
is immersed in liquid nitrogen, the in-situ wrapping of Fe3O4 nanoparticles with GNSs is easily realized. The structural
conversion is closely correlated with the initial temperature of mixed
suspension, the zeta potential of Fe3O4 nanoparticles
and the immersion way. Remarkably, such hybrid structure provides
the right combination of electrode properties for high-performance
lithium-ion batteries. Compared with other wrapping structure, such
1D wrapping structure (GNSs wrapping) effectively limits the volume
expansion of Fe3O4 nanoparticles during the
cycling process, consequently, a high reversible capacity, good rate
capability, and excellent cyclic stability are achieved with the material
as anode for lithium storage. The results presented here may pave
a way for the large-scale preparation of GNS-based materials in electrochemical
energy storage applications.
The utilization of porous carbon frameworks as hosts for sulfur loading is an important theme in current Li‐S battery research. Unfortunately, the high loading of insulating sulfur often leads to low specific capacities, poor rate properties, and rapid capacity loss. To address this challenge, a facile templating route to fabricate a novel host material, hierarchical porous carbon rods constructed by vertically oriented porous graphene‐like nanosheets (HPCR) is presented. With a high specific surface area, ultralarge pore volume, hierarchical porous structures, and ideal ion transfer pathways, HPCR is a promising candidate for high sulfur loading. When used as the active material for a sulfur cathode, the HPCR‐S composite with 78.9 wt% sulfur exhibits excellent rate performance (646 mAh g−1sulfur at 5 C) and cycling stability (700 mAh g−1sulfur after 300 cycles at 1 C). Even with a sulfur content of 88.8 wt%, the HPCR‐S composite, without any additional protective polymer coating, still delivers a good rate performance (545 mAh g−1sulfur at 3 C) and cycling stability (632 mAh g−1sulfur after 200 cycles at 1 C). More importantly, the high sulfur loading (88.8 wt%) ensures that the HPCR‐S composite has a high energy density (880 mAh cm−3cathode after 200 cycles at 1 C).
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