Rational cathode configuration with bilayer membranes to engineer current-collector-free high-areal-sulfur lithium-sulfur batteries

The application of light-weight current collectors is preferred because of the increased energy density of the batteries.Bearing it in mind,the cathode is designed with self-made paperlike memberane as current collector coupled with another interlayer to enable the high-energy-density lithium-sulfur batteries.Via a facile and green step-by-step methodology,the hybrid membrane is finalized successfully,consisting of reduced graphene oxide sheets covering paper-derived carbon(GPC)bearing Fe@Fe2O3 and Fe1−xS@Fe2O3 core-shell nanoparticles(FeFeO/FeSFeO@GPC).The film works as the current collector and interlayer simultaneously considering the porous and conductive features.As demonstrated by the electrochemical testing,the FeFeO/FeSFeO@GPC hybrid cell exhibits attractive cycling stability and superior rate capability.The cell configuration and structural/composition merits of FeFeO/FeSFeO@GPC film facilitate the faster reaction kinetics,conducive to the improvement of capacity retention.In view of the effective cathode design,the areal sulfur loading is increased to 10.46 mg·cm^(−2)and a reversible capacity of 6.67 mAh·cm^(−2)can be retained after 60 cycles at 0.1 C.

Towards full demonstration of high areal loading sulfur cathode in lithium–sulfur batteries

Lithium–sulfur(Li–S)batteries have been recognized as promising substitutes for current energy-storage technologies owing to their exceptional advantages in very high-energy density and excellent material sustainability.The cathode with high sulfur areal loading is vital for the practical applications of Li–S batteries with very high energy density.However,the high sulfur loading in an electrode results in poor rate and cycling performances of batteries in most cases.Herein,we used diameters of 5.0(D5)and 13.0(D13)mm to probe the effect of electrodes with different sizes on the rate and cycling performances under a high sulfur loading(4.5 mg cm^-2).The cell with D5 sulfur cathode exhibits better rate and cycling performances comparing with a large(D13)cathode.Both the high concentration of lithium polysulfides and corrosion of lithium metal anode impede rapid kinetics of sulfur redox reactions,which results in inferior battery performance of the Li–S cell with large diameter cathode.This work highlights the importance of rational matching of the large sulfur cathode with a high areal sulfur loading,carbon modified separators,organic electrolyte,and Li metal anode in a pouch cell,wherein the sulfur redox kinetics and lithium metal protection should be carefully considered under the flooded lithium polysulfide conditions in a working Li–S battery.

Separator coatings as efficient physical and chemical hosts of polysulfides for high-sulfur-loaded rechargeable lithium–sulfur batteries

Lithium-sulfur batteries(LSBs)are promising alternative energy storage devices to the commercial lithium-ion batteries.However,the LSBs have several limitations including the low electronic conductivity of sulfur(5×10^-30S cm^-1),associated lithium polysulfides(PSs),and their migration from the cathode to the anode.In this study,a separator coated with a Ketjen black(KB)/Nafion composite was used in an LSB with a sulfur loading up to 7.88 mg cm^-2to mitigate the PS migration.A minimum specific capacity(Cs)loss of 0.06%was obtained at 0.2 C-rate at a high sulfur loading of 4.39 mg cm^-2.Furthermore,an initial areal capacity up to 6.70 mAh cm^-2 was obtained at a sulfur loading of 7.88 mg cm^-2.The low Cs loss and high areal capacity associated with the high sulfur loading are attributed to the large surface area of the KB and sulfonate group(SO3^-)of Nafion,respectively,which could physically and chemically trap the PSs.

石墨烯包覆的硫填充碳纳米笼自支撑整体材料的制备及其锂硫电池性能研究

锂硫电池具有理论能量密度高、活性物质价廉、毒性低等优点,是最具发展潜力的高能量二次电池之一,其应用仍存在硫面载量小、循环寿命短和库伦效率低等难题.制备了石墨烯包覆的硫填充碳纳米笼自支撑整体材料,可直接用作锂硫电池正极,避免使用粘结剂、导电剂和集流体,当硫的面载量为3.8 mg·cm^(-2)时,锂硫电池展现出高的可逆比容量(1104 mAh·g^(-1))、优异的循环稳定性(每圈容量衰减率仅为0.049%@1.0 A·g^(-1))和>99.9%的库伦效率,其面积比容量(3.7 mAh·cm^(-2))处于锂硫电池的先进水平.该电极的优异性能可归因于以下因素的协同作用:碳纳米笼的物理限域作用及石墨烯中含氧官能团的化学吸附作用有效抑制了活性物质的流失,微孔-介孔-大孔共存的分级孔结构和高导电性利于离子和电子的传输,纳米笼空腔填充有利于缓解体积膨胀造成的影响,整体材料的自支撑稳定结构有利于增加硫载量且维持电化学性能.本研究还提供了一种工艺简单、能有效提高面积比容量的硫正极制备方法.