Energy Storage Materials for Solid‐State Batteries: Design by Mechanochemistry

Abstract

Commercialization of solid‐state batteries requires the upscaling of the material syntheses as well as the mixing of electrode composites containing the solid electrolyte, cathode active materials, binders, and conductive additives. Inspired by recent literature about the tremendous influence of the employed milling and dispersing procedure on the resulting ionic transport properties of solid ionic conductors and the general performance of all solid‐state batteries, in this review, the underlying physical and mechanochemical processes that influence this processing are discussed. By discussing and combining the theoretical backgrounds of mechanical milling with regard to mechanochemical synthesis and dispersing of particles together with a wide range of examples, a better understanding of the critical parameters attached to mechanical milling of solid electrolytes and solid‐state battery components is provided.

In Search of the Best Solid Electrolyte-Layered Oxide Pairing for Assembling Practical All-Solid-State Batteries

“…22 Moreover, their chemical-physical properties were also shown to depend on their synthesis method, either via solvent assisted reactions involving precipitation/crystallization in organic solvents, high temperature solid-state reactions (>500 °C) or mechanical ball milling followed by annealing steps. [23][24][25][26] Among them, the solvent-based routes appear to be particularly attractive for solid electrolyte (SE) -CAM composite preparation in a core-shell like structure (namely SE-coated oxide) by maximizing the energy density at electrode level while enhancing ionic percolation and boosting the cell performance. [27][28][29] However, in practice, such solution processes were shown to lead to phase contaminations or surficial remaining solvent species on solid ionic conductors.…”

Challenges, interface engineering, and processing strategies toward practical sulfide‐based all‐solid‐state lithium batteries

“…46,48,162 However, as we discussed previously, the direct scalability in these conventional routes is still questionable because they are time-intensive, output-limit, and energy-consuming. 342,343 In 2013, the first report of the low-temperature synthesis of β-Li 3 PS 4 by wet-chemistry route provided a promising prospect for the actual scale application of sulfide SEs. 344 Compared with solid-state syntheses and mechanochemical syntheses, the wet synthesis for sulfide SEs presents several significant advantages as follows in terms of shortening reaction time, producing homogeneous materials and convenient cell integration as well as scalability:…”

Garnet to hydrogarnet: effect of post synthesis treatment on cation substituted LLZO solid electrolyte and its effect on Li ion conductivity

“… 11 It is assumed, that a maximum of sublattice entropy in garnet-type structures could have an enhancing effect on the Li + conductivity. 10 The introduction of defects and distortions via ball milling can have a positive effect on conductivity, as explained by Schlem et al 12 Liu et al follow this by stating that an understanding of this local defect structure is also important in order to prevent dendrite formation. 13 Thorough choice of the substituents allows tuning the materials properties and gaining more efficient sintering conditions and thus economic fabrication for industrial application.…”