An in situ constructed VO2–VN binary host was realized to accomplish smooth immobilization–diffusion–conversion of polysulfides, targeting high-sulfur-load Li–S batteries.
The ever-growing demand for high-energy and long-life energy storage devices has spurred extensive research beyond conventional lithium-ion battery systems. Amongst these, rechargeable lithium-sulfur (Li-S) batteries, as a promising next-generation energy storage technology, have captured vast interest because of the high capacity (1672 mAh g −1 ), large abundance of sulfur, and environmental compatibility. [1][2][3][4] Although there has been significant advance by far in designing state-of-theart Li-S batteries, their practical utilization and large-scale commercialization are still impeded by a multitude of technological obstacles, namely, i) the insulating nature of S/Li 2 S that would jeopardize the overall conductivity of the electrode and hence affect the utilization of sulfur; ii) the shuttle effect induced by the dissolution and diffusion of lithium polysulfide that could lead to a rapid capacity fading; and iii) the considerable volume expansion of the sulfur cathode upon cycling. [5,6] To tackle these issues, great efforts have been devoted to developing appropriate host materials in combination with optimizing the cathode architectures toward advanced Li-S batteries. A ubiquitously employed strategy is to encapsulate sulfur and/or polysulfides with the aid of porous carbonaceous materials, such as carbon nanotubes, [1,[7][8][9][10] hollow carbon spheres, [11,12] and graphene, [13][14][15] aiming to attain enhanced electrode conductivity, improved sulfur utilization, and buffered volume change. However, this has been proved to be far from ideal, owing to weak van der Waals (vdW) interaction between nonpolar carbon and polar polysulfide species that only gives rise to a physical confinement, insufficient to alleviate the polysulfide shuttle over a long lifespan. In this regard, the introduction of polar nanomaterials (e.g., transition metal oxides, [16][17][18] sulfides, [19][20][21] and nitrides [22,23] ) within the sulfur host has witnessed an efficient suppression of shuttle effect, where polysulfides are chemically anchored onto these polar species. Nevertheless, the limited electrical conductivity of most metal oxides/sulfides would otherwise result in sluggish kinetics of polysulfide redox reactions, inevitably causing poor rate capability and fast capacity decay. Latest investigations have revealed that the integration of polar nanocrystals/nanosheets Lithium-sulfur (Li-S) batteries are deemed to be one of the most promising energy storage technologies because of their high energy density, low cost, and environmental benignancy. However, existing drawbacks including the shuttling of intermediate polysulfides, the insulating nature of sulfur, and the considerable volume change of sulfur cathode would otherwise result in the capacity fading and unstable cycling. To overcome these challenges, herein an in situ assembly route is presented to fabricate VS 2 /reduced graphene oxide nanosheets (G-VS 2 ) as a sulfur host. Benefiting from the 2D conductive and polar VS 2 interlayered within a graphene fra...
Aqueous electrolytes offer major advantages in safe battery operation, green economy, and low production cost for advanced battery technology. However, strong water activity in aqueous electrolytes provokes a hydrogen evolution reaction and parasitic passivation on electrodes, leaving poor ion‐transport in the electrolyte/electrode interface. Herein, a zeolite molecular sieve‐modified (zeolite‐modified) aqueous electrolyte is proposed to reduce water activity and its side‐reaction. First, Raman spectroscopy reveals a highly aggressive solvation configuration and significantly suppressed water activity toward single water molecule. Then less hydrogen evolution and anti‐corrosion ability of zeolite‐modified electrolyte by simulation and electrochemical characterizations are identified. Consequently, a zinc (Zn) anode involves less side‐reaction, and develops into a compact deposition morphology, as proved by space‐resolution characterizations. Moreover, zeolite‐modified electrolyte favors cyclic life of symmetric Zn||Zn cells to 4765 h at 0.8 mA cm−2, zinc‐VO2 coin cell to 3000 cycles, and pouch cell to 100 cycles. Finally, the mature production technique and low‐cost of zeolite molecular sieve would tremendously favor the future scale‐up application in engineering aspect.
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