Abstract:Herein an effective way for construction of all-solid-state lithium-sulfur batteries (LSBs) with sulfur/reduced graphene oxide (rGO) and Li Si P S Cl solid electrolyte is reported. In the composite cathode, the Li Si P S Cl powder is homogeneously mixed with the S/rGO composite to enhance the ionic conductivity. Coupled with a metallic Li anode and solid electrolyte, the designed S/rGO-Li Si P S Cl composite cathode exhibits a high specific capacity and good cycling stability. A high initial discharge capacity… Show more
“…Results (Supplementary Figure 10) show that LSPS 460 has the highest ionic conductivity of 3.1 mS cm −1 , while LSPS 400 and 480 show relatively lower ionic conductivity of 2.28 and 2.39 mS cm −1 , respectively. Note that even higher ionic conductivity may be obtained by applying higher pressure 27 during the impedance measurement, which was not applied during our test (see Methods).Fig. 4Battery performance of Li 4 Ti 5 O 12 +LSPS-Cl+C/LSPS-Cl/glass fiber/Li cells incorporating different LSPS-Cl materials annealed at different temperatures.…”
Section: Resultsmentioning
confidence: 99%
“…Despite the superior lithium-ion conductivity of LGPS and LSPS 13,16,23,24 , various groups 23–26 reported the narrower stability windows of around 1.7−2.1 V, while others reported wider voltage windows 13,16,27 . We suggest that changes in the microstructure of the electrolyte materials or in the volume constriction condition of the battery cells may result in different voltage stability windows.…”
Solid electrolyte is critical to next-generation solid-state lithium-ion batteries with high energy density and improved safety. Sulfide solid electrolytes show some unique properties, such as the high ionic conductivity and low mechanical stiffness. Here we show that the electrochemical stability window of sulfide electrolytes can be improved by controlling synthesis parameters and the consequent core-shell microstructural compositions. This results in a stability window of 0.7–3.1 V and quasi-stability window of up to 5 V for Li-Si-P-S sulfide electrolytes with high Si composition in the shell, a window much larger than the previously predicted one of 1.7–2.1 V. Theoretical and computational work explains this improved voltage window in terms of volume constriction, which resists the decomposition accompanying expansion of the solid electrolyte. It is shown that in the limiting case of a core-shell morphology that imposes a constant volume constraint on the electrolyte, the stability window can be further opened up. Advanced strategies to design the next-generation sulfide solid electrolytes are also discussed based on our understanding.
“…Results (Supplementary Figure 10) show that LSPS 460 has the highest ionic conductivity of 3.1 mS cm −1 , while LSPS 400 and 480 show relatively lower ionic conductivity of 2.28 and 2.39 mS cm −1 , respectively. Note that even higher ionic conductivity may be obtained by applying higher pressure 27 during the impedance measurement, which was not applied during our test (see Methods).Fig. 4Battery performance of Li 4 Ti 5 O 12 +LSPS-Cl+C/LSPS-Cl/glass fiber/Li cells incorporating different LSPS-Cl materials annealed at different temperatures.…”
Section: Resultsmentioning
confidence: 99%
“…Despite the superior lithium-ion conductivity of LGPS and LSPS 13,16,23,24 , various groups 23–26 reported the narrower stability windows of around 1.7−2.1 V, while others reported wider voltage windows 13,16,27 . We suggest that changes in the microstructure of the electrolyte materials or in the volume constriction condition of the battery cells may result in different voltage stability windows.…”
Solid electrolyte is critical to next-generation solid-state lithium-ion batteries with high energy density and improved safety. Sulfide solid electrolytes show some unique properties, such as the high ionic conductivity and low mechanical stiffness. Here we show that the electrochemical stability window of sulfide electrolytes can be improved by controlling synthesis parameters and the consequent core-shell microstructural compositions. This results in a stability window of 0.7–3.1 V and quasi-stability window of up to 5 V for Li-Si-P-S sulfide electrolytes with high Si composition in the shell, a window much larger than the previously predicted one of 1.7–2.1 V. Theoretical and computational work explains this improved voltage window in terms of volume constriction, which resists the decomposition accompanying expansion of the solid electrolyte. It is shown that in the limiting case of a core-shell morphology that imposes a constant volume constraint on the electrolyte, the stability window can be further opened up. Advanced strategies to design the next-generation sulfide solid electrolytes are also discussed based on our understanding.
“…Besides volume expansion during lithiation is another challenge of sulfur to be utilized in LIBs. Combining sulfur with reducedgraphene oxide(rGO) is shown to have better results mainly because rGO easily hosts the volume expansion of sulfur . The composite cathode should also be ionically conductive.…”
Section: Introductionmentioning
confidence: 99%
“…Combining sulfur with reducedgraphene oxide(rGO) is shown to have better results mainly because rGO easily hosts the volume expansion of sulfur. [12] The composite cathode should also be ionically conductive. Combining rGO/Sulfur composites with ionically conductive solid electrolytes not only makes cathodes conductive but also decrease the chemical potential difference between the electrode and electrolyte.…”
The construction of all‐solid‐state batteries is now easier after the successful synthesis of sulfur‐based solid electrolytes with extremely high ionic conductivities. Utilizing lithium metal as the anode in these batteries requires a protective solid electrolyte layer to prevent corrosion due to the highly reactive nature of lithium. Li3N coating on lithium metal is a promising way of preventing the degradation of the electrolyte during charge and discharge. In this study, utilization of a Li3N‐coated lithium anode and Li7P3S11 solid electrolyte are reported, where a quaternary reduced graphene oxide (rGO)/S/carbon black/Li7P3S11 composite is used as cathode in the assembled cell. Our results indicate that protecting the Li metal with a Li3N coating does not affect the electrochemical characteristics of the cell and extends the cycle life of the battery. A cell assembled with a protective layer was shown to having 306 mAh g−1 capacity after 120 cycles at 160 mAh g−1 current density, whereas a cell without protective layer had a capacity of 260 mAh g−1.
“…To be applied in solid‐state batteries, sulfide solid electrolytes are typically used in the form of powder. For example, mixtures of active material powders, solid electrolyte powders and carbon are widely used as composite cathodes . In addition, pellets cold‐pressed from the solid electrolyte powders are used as the ion‐transport layers which separate the anode and the cathode .…”
The interfacial resistance and capacitance in pellets made from GeS2‐Ga2S3‐Li2S‐LiI glass powder are studied under uniaxial compression. By varying the pressure, remarkable change in the geometric dimension of the interfacial resistance and capacitance is observed. Assuming that the interfacial resistance and capacitance arise from the contact region between the powder particles, a quantitative model is established that well describes the geometric dimension change in the interfacial resistance and capacitance. This work emphasizes that ameliorating the contact between the particles is one of the most important methods to reduce the interfacial resistance in the powder‐type ionic‐conduction devices made from highly‐conductive sulfide solid electrolyte powders.
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