Enabling all-solid-state Li-ion batteries requires solid electrolytes with high Li ionic conductivity and good electrochemical stability.F ollowing recent experimental reports of Li 3 YCl 6 and Li 3 YBr 6 as promising new solid electrolytes,weused first principles computation to investigate the Li-ion diffusion, electrochemical stability,a nd interface stability of chloride and bromide materials and elucidated the origin of their high ionic conductivities and good electrochemical stabilities.Chloride and bromide chemistries intrinsically exhibit lowmigration energy barriers,wide electrochemical windows,a nd are not constrained to previous design principles for sulfide and oxide Li-ion conductors,allowing for muchg reater freedom in structure,c hemistry,c omposition, and Li sublattice for developing fast Li-ion conductors.O ur study highlights chloride and bromide chemistries as apromising new researchdirection for solid electrolytes with high ionic conductivity and good stability.All-solid-state lithium-ion batteries (ASBs) with inorganic lithium solid electrolytes (SEs) are regarded as promising next-generation energy storage devices.ASBs solve the safety issue caused by the flammability of organic liquid electrolyte and potentially provide higher energy density with Li metal anode and high-voltage cathode materials. [1] However,i th as been ag reat challenge to develop solid-state Li-ion conductors with high Li + conductivity at room temperature comparable to that of liquid electrolytes and with good electrochemical stability for Li-ion batteries with avoltage of > 4V .C urrent research efforts on solid-state Li-ion conductors focus mostly on oxides and sulfides. [1a,b,2] Unfortunately, oxide and sulfide chemistries have an undesirable trade-off between ionic conductivity and stability.S ulfide-based solidstate Li-ion conductors such as Li 10 GeP 2 S 12 (LGPS) andSupportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.Figure 3. Calculated thermodynamics intrinsic electrochemical windows of Li-M-X ternary fluorides, chlorides, bromides, iodides, oxides, and sulfides. Mi sametal cation at its highest commonv alence state.

Ceramics are an important class of materials with widespread applications because of their high thermal, mechanical, and chemical stability. Computational predictions based on first principles methods can be a valuable tool in accelerating materials discovery to develop improved ceramics. It is essential to experimentally confirm the material properties of such predictions. However, materials screening rates are limited by the long processing times and the poor compositional control from volatile element loss in conventional ceramic sintering techniques. To overcome these limitations, we developed an ultrafast high-temperature sintering (UHS) process for the fabrication of ceramic materials by radiative heating under an inert atmosphere. We provide several examples of the UHS process to demonstrate its potential utility and applications, including advancements in solid-state electrolytes, multicomponent structures, and high-throughput materials screening.

Since the first demonstration of prototype Li batteries (TiS 2 /Li) in 1976, [1] the develo pment of LIBs to date has been strongly affected by safety issues. One of the major technical breakthroughs for the commer cialization of LIBs was the replacement of Li metal with carbonaceous materials as the anode. [2][3][4] It is well known that the use of Li metal was challenged by serious safety concerns associated with internal short circuit by the dendritic growth of Li metal. [5][6][7] The everrising requirements for higher energy density of LIBs have raised more serious safety concerns. Raising the upper cutoff voltages leads to poorer sta bility at electrode-electrolyte interfaces. [8,9] Ultrathinning the polymeric separators to less than 10 µm, despite the reinforce ments using ceramic materials, [10][11][12] result in more vulnerability toward internal short circuits. These may also be related to degassing, fire, and explosion accidents of LIBs in recent years. Further more, largescale applications of LIBs, such as batterydriven electric vehicles and gridscale energy storages, face unprecedented challenges in terms of safety requirements. [13][14][15] In this regard, solidification of conventional flammable organic liquid electrolytes with inorganic materials, such as superionic conductor solid electrolytes (SEs), is an ideal solution. [16][17][18][19][20][21][22][23][24][25] Another strong motivation in the development of SEs is to unleash the harness of limited energy density for con ventional LIBs by using SEs to stabilize and enable alternative highcapacity electrode materials, such as Li metal anode and sulfur cathode. [15,23] Additionally, the design of allsolidstate Li or Liion batteries (ALSBs) by stacking bipolar electrodes allows the minimization of inactive encasing materials, thereby increasing celllevel energy density. [22,26] The first superionic conductors PbF 2 and Ag 2 S were discov ered by Michael Faraday in 1838. [27] Since then, several notable progresses in the field of solidstate superionic conductors and their newly enabled electrochemical devices had occurred; [27] the development of oxygenion conductors (Ydoped ZrO 2 ) applied to solid oxide fuel cells, the discoveries of Ag + superionic conduc tors (e.g., RbAg 4 I 5 ), and the development of Naion conducting sodium beta alumina (β″Al 2 O 3 ). Currently, it is a promi sing opportunity for Liion SEs to revolutionize LIB technologies Owing to the ever-increasing safety concerns about conventional lithium-ion batteries, whose applications have expanded to include electric vehicles and grid-scale energy storage, batteries with solidified electrolytes that utilize nonflammable inorganic materials are attracting considerable attention. In particular, owing to their superionic conductivities (as high as ≈10 −2 S cm −1 ) and deformability, sulfide materials as the solid electrolytes (SEs) are considered the enabling material for high-energy bulk-type all-solid-state batteries. Herein the authors provide a brief review on recent progress in sulf...

The all-solid-state lithium-ion battery is a promising next-generation battery technology. However, the realization of all-solid-state batteries is impeded by limited understanding of solid electrolyte materials and solid electrolyte-electrode interfaces. In this review, we present an overview of recently developed computation techniques and their applications in understanding and advancing materials and interfaces in all-solid-state batteries. We review the role of ab initio molecular dynamics simulations in studying fast ion conductors and discuss the capabilities of thermodynamic calculations powered by materials databases for identifying the chemical and electrochemical stability of solid electrolyte materials and solid electrolyte-electrode interfaces. We highlight the computational studies in the design and discovery of new solid electrolyte materials and outline design guidelines for solid electrolytes and their interfaces. We conclude with discussion of future directions in computation techniques, materials development, and interface engineering for all-solid-state lithium-ion batteries.

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