Ultrathin MnO2/Graphene Oxide/Carbon Nanotube Interlayer as Efficient Polysulfide‐Trapping Shield for High‐Performance Li–S Batteries
TL;DR: In this paper, a simple layer-by-layer procedure is used to construct a sandwiched vein-membrane interlayer of thickness 2 µm and areal density 0.104 mg cm−2 by loading MnO2 nanoparticles and graphene oxide (GO) sheets on superaligned carbon nanotube films.
Abstract: Ultrathin MnO2/graphene oxide/carbon nanotube (G/M@CNT) interlayers are developed as efficient polysulfide-trapping shields for high-performance Li–S batteries. A simple layer-by-layer procedure is used to construct a sandwiched vein–membrane interlayer of thickness 2 µm and areal density 0.104 mg cm−2 by loading MnO2 nanoparticles and graphene oxide (GO) sheets on superaligned carbon nanotube films. The G/M@CNT interlayer provides a physical shield against both polysulfide shuttling and chemical adsorption of polysulfides by MnO2 nanoparticles and GO sheets. The synergetic effect of the G/M@CNT interlayer enables the production of Li–S cells with high sulfur loadings (60–80 wt%), a low capacity decay rate (−0.029% per cycle over 2500 cycles at 1 C), high rate performance (747 mA h g−1 at a charge rate of 10 C), and a low self-discharge rate with high capacity retention (93.0% after 20 d rest). Electrochemical impedance spectroscopy, cyclic voltammetry, and scanning electron microscopy observations of the Li anodes after cycling confirm the polysulfide-trapping ability of the G/M@CNT interlayer and show its potential in developing high-performance Li–S batteries.
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TL;DR: In this article, a twinborn TiO2-TiN heterostructure was proposed to improve the performance of Li-S batteries by combining the merits of highly adsorptive TiO 2 with conducting TiN and achieving smooth trapping-diffusion-conversion of LiPSs across the interface.
Abstract: The practical use of lithium–sulfur (Li–S) batteries is largely hindered by their poor cycling stability because of the shuttling of soluble lithium polysulfides (LiPSs) in a slow redox reaction. Physical and chemical confinement by carbon or noncarbon hosts has been used to block LiPS shuttling, but this may only be a complete solution to the problem if it combines with LiPS fast conversion into an insoluble sulfide. Here we report a twinborn TiO2–TiN heterostructure that combines the merits of highly adsorptive TiO2 with conducting TiN and achieves smooth trapping–diffusion–conversion of LiPSs across the interface. TiO2 has high adsorption for LiPSs while TiN promotes their conversion into insoluble Li2S. The fast diffusion of LiPSs from TiO2 to TiN helps achieve both high trapping efficiency and fast conversion. By loading such a heterostructure onto graphene, which acts as a physical barrier, a compact and thin coating is fabricated on the separator, and LiPS shuttling is greatly restrained even with a high sulfur loading. A capacity of 927 mA h g−1 after 300 cycles is obtained under a low current density of 0.3C. Over 2000 cycles, capacity retentions of 73% and 67% at 1C are achieved for sulfur loadings of 3.1 and 4.3 mg cm−2. Such an interlayer is expected to promote the practical use of Li–S batteries because of the simple processing and the resulting outstanding capacity and cyclic performance. Such a heterostructure suggests a new way to produce multifunctional interlayers that improve the performance of energy storage devices.
818 citations
TL;DR: In this article, a review of the advanced interlayer systems is presented, and the operating mechanisms and widespread availability of interlayers in lithium-sulfur batteries are concluded.
340 citations
TL;DR: In this paper, a unique sulfur host hybrid material comprising nanosized nickel sulfide (NiS) uniformly distributed on 3D carbon hollow spheres (C-HS) is fabricated using an in situ thermal reduction and sulfidation method.
Abstract: Lithium–sulfur batteries are a promising next-generation energy storage device owing to their high theoretical capacity and the low cost and abundance of sulfur. However, the low conductivity and loss of active sulfur material during operation greatly limit the rating capabilities and cycling stability of lithium–sulfur batteries. In this work, a unique sulfur host hybrid material comprising nanosized nickel sulfide (NiS) uniformly distributed on 3D carbon hollow spheres (C-HS) is fabricated using an in situ thermal reduction and sulfidation method. In the hybrid material, the nanosized NiS provides a high adsorption capability for polysulfides and the C-HS serves as a physical confinement for polysulfides and also a 3D electron transfer pathway. Moreover, NiS has strong chemical coupling with the C-HS, favoring fast charge transfer and redox kinetics of the sulfur electrode. With a sulfur loading of up to 2.3 mg cm−2, the hybrid material-based lithium–sulfur batteries offer a capacity decay as low as 0.013% per cycle and a capacity of 695 mA h g−1 at 0.5 C after 300 cycles. This unique 3D hybrid material with strong chemical coupling provides a promising sulfur host for high performance lithium–sulfur batteries.
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TL;DR: In this article, the synthesis of a graphene-sulfur composite material by wrapping poly(ethylene glycol) (PEG) coated submicrometer sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles was reported.
Abstract: We report the synthesis of a graphene–sulfur composite material by wrapping poly(ethylene glycol) (PEG) coated submicrometer sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles. The PEG and graphene coating layers are important to accommodating volume expansion of the coated sulfur particles during discharge, trapping soluble polysulfide intermediates, and rendering the sulfur particles electrically conducting. The resulting graphene–sulfur composite showed high and stable specific capacities up to ∼600 mAh/g over more than 100 cycles, representing a promising cathode material for rechargeable lithium batteries with high energy density.
2,013 citations