High grain-boundary resistance, Li-dendrite formation, and electrode/Li interfacial resistance are three major issues facing garnet-based solid electrolytes. Herein, interfacial architecture engineering by incorporating 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl) imide (BMP-TFSI) ionic liquid into a garnet oxide is proposed. The “soft” continuous BMP-TFSI coating with no added Li salt generates a conducting network facilitating Li+ transport and thus changes the ion conduction mode from point contacts to face contacts. The compacted microstructure suppresses Li-dendrite growth and shows good interfacial compatibility and interfacial wettability toward Li metal. Along with a broad electrochemical window larger than 5.5 V and an Li+ transference number that practically reaches unity, LiNi0.8Co0.1Mn0.1O2/Li and LiFePO4/Li solid-state batteries with the hybrid solid electrolyte exhibit superior cycling stability and low polarization, comparable to those with commercial liquid electrolytes, and excellent rate capability that is better than those of Li-salt-based ionic-liquid electrolytes.@en

Li6PS5X (X = Cl, Br, I) argyrodites possess high ionic conductivity but with rather scattered values due to various processing conditions. In this work, Li6PS5X solid electrolytes were prepared by solid-state sintering or mechanical alloying and optimized with or without excess Li2S. Solid-state sintering prefers excess Li2S, whereas mechanical alloying prefers stoichiometric Li2S to synthesize high-purity samples with high ionic conductivity. Solid-state sintering is also more suitable than mechanical milling for high ionic conductivity. Li6PS5Cl with the highest ionic conductivity among Li6PS5X was comprehensively characterized for electrochemical performance and air stability. MoS2/Li6PS5Cl all-solid-state batteries assembled with Li6PS5Cl-coated MoS2 as cathode and with Li6PS5Cl as solid electrolyte demonstrate high capacity and good cycling stability.@en

Exploration of advanced anode materials is a highly relevant research topic for next generation lithium-ion batteries. Here, we report severe lattice distorted MoS2 nanosheets with a flower-like morphology prepared with PEG400 as additive, which acts not only as surfactant but importantly, also as reactant. Notably, in the absence of a carbon-related incorporation/decoration, it demonstrates superior electrochemical performance with a high reversible capacity, a good cycling stability, and an excellent rate capability, originated from the advantages of synthesized MoS2 including enlarged interlayer spacing, 1T-like metallic behavior, and coupling of Mo–O–C (and Mo–O) hetero-bonds. PEG-assisted synthesis is believed applicable to other anode materials with a layered structure for lithium-ion batteries.@en

Sulfide solid electrolytes possess high ionic conductivity and moderate dendrite suppression capability, but rather poor compatibility against oxide cathodes and metallic Li. Here, we report O-doped Li6PS5Br as solid electrolyte synthesized by a facile solid-state sintering. Different from other O-incorporated sulfides, the O atoms in Li6PS5-xOxBr prefer to substitute the S atoms at free S2− sites rather than those at the PS4 tetrahedra. Remarkably, without deteriorating the ionic conductivity, this inorganic solid electrolyte with O doping exhibits comprehensively enhanced properties including excellent dendrite suppression capability, superior electrochemical and chemical stability against Li metal as well as high voltage oxide cathodes, and good air stability. Li(Ni0.8Co0.1Mn0.1)O2 and LiCoO2-based all-solid-state batteries with Li6PS4.7O0.3Br electrolyte deliver high specific capacity, superior rate capability, and outstanding cycling stability accompanied with low interfacial resistivity. This type of inorganic solid electrolytes is promising for all-solid-state batteries with high energy density.@en

Based on its high Li-ion conductivity, argyrodite Li6PS5Br is a promising solid electrolyte for all-solid-state batteries. However, more understanding is required on the relation between the solid electrolyte conductivity and the solid-state battery performance with the argyrodite structure, crystallinity and particle size that depend on the synthesis conditions. In the present study, this relationship is investigated using neutron and X-ray diffraction to determine the detailed structure and impedance as well as 7Li solid state NMR spectroscopy to study the Li-ion kinetics. It is found that depending on the synthesis conditions the distribution of the Br dopant over the crystallographic sites in Li6PS5Br is inhomogeneous, and that this may be responsible for a larger mobile Li-ion fraction at the interface regions in the annealed argyrodite materials. Comparing the bulk and interface properties of the differently prepared Li6PS5Br materials, it is proposed that optimal solid-state battery performance requires a different particle size for the solid electrolyte only region and the solid electrolyte in the cathode mixture. In the electrolyte region, the grain boundary resistance is minimized by annealing the argyrodite Li6PS5Br resulting in relatively large crystallites. In the cathode mixture however, additional particle size reduction of the Li6PS5Br is required to provide abundant Li6PS5Br-Li2S interfaces that reduce the resistance of this rate limiting step in Li-ion transport. Thereby the results give insight in how to improve solidstate battery performance by controlling the solid electrolyte structure. @en

It is a highly relevant topic concerning how to improve the electrochemical performance of anode materials for the next generation lithium-ion batteries (LIBs). Herein, for the first time, we report a facile and controllable approach to modify MoS 2 nanosheets, a typical 2D material, as an anode material for advanced LIBs via oxygen plasma engineering. An oxygen plasma treatment not only generates vacancies/defects but also incorporates heteroatom doping to form Mo–O–C bonds. This unique hybrid specialty enables the oxygen-plasma-treated MoS 2 to achieve superior electrochemical performance with high reversible capacities, a long-term cycle life, and good rate capabilities. The plasma-assisted modification is believed to be applicable for other 2D materials as an efficient anode for energy storages. @en