Amorphous Materials for Lithium‐Ion and Post‐Lithium‐Ion Batteries

Abstract

Lithium‐ion and post‐lithium‐ion batteries are important components for building sustainable energy systems. They usually consist of a cathode, an anode, an electrolyte, and a separator. Recently, the use of solid‐state materials as electrolytes has received extensive attention. The solid‐state electrolyte materials (as well as the electrode materials) have traditionally been overwhelmingly crystalline materials, but amorphous (disordered) materials are gradually emerging as important alternatives because they can increase the number of ion storage sites and diffusion channels, enhance solid‐state ion diffusion, tolerate more severe volume changes, and improve reaction activity. To develop superior amorphous battery materials, researchers have conducted a variety of experiments and theoretical simulations. This review highlights the recent advances in using amorphous materials (AMs) for fabricating lithium‐ion and post‐lithium‐ion batteries, focusing on the correlation between material structure and properties (e.g., electrochemical, mechanical, chemical, and thermal ones). We review both the conventional and the emerging characterization methods for analyzing AMs and present the roles of disorder in influencing the performances of various batteries such as those based on lithium, sodium, potassium, and zinc. Finally, we describe the challenges and perspectives for commercializing rechargeable AMs‐based batteries.

Crystallography of Active Particles Defining Battery Electrochemistry

“…Strain can also be induced by the distortion of manganese containing active materials due to the Jahn Teller effect [49] and the amorphization of active material creating heterogeneous crystallographic structures within active material particles making them more susceptible to mechanical degradation. [50]…”

Effects of Nonequilibrium Atomic Structure on Ionic Diffusivity in LLZO: A Classical and Machine Learning Molecular Dynamics Study

“…Recently, there has been increased interest in understanding the effects of nonequilibrium motifs such as grain boundaries, amorphous phases, and highly strained regions, which appear to have nonnegligible impacts both on diffusion and stability. 2,10,11 For instance, the effect of the grain structure and grain boundaries on ionic conductivity has been tested by both experiment 12,13 and computation. 14−17 These investigations have confirmed the negative impact on diffusion of atomic-scale structural disorder.…”

“…In many cases, such regions can ultimately dictate properties, performance, and lifetime of functional materials and devices. For instance, amorphous materials in energy storage devices have been shown to have desirable elastomechanical properties, 1,2 improved processability, 1,2 and better interfacial coherence and electronic properties. 3,4 From a computational perspective, atomically disordered and strained materials have historically been especially challenging to simulate, as they require large simulation cells and many configurations for proper sampling.…”

“…In many cases, such regions can ultimately dictate properties, performance, and lifetime of functional materials and devices. For instance, amorphous materials in energy storage devices have been shown to have desirable elastomechanical properties, , improved processability, , and better interfacial coherence and electronic properties. , …”

“…Diffusivity [cm2 /s] in Amorphous LLZO at 700 K with 112%V exp (ρ = 4.52 g/cm 3 ) from a Computational Experiment that Uses a Different Potential to Generate the Structure than the One Used to Run the MD a CIP CIP ratio is the given diffusivity over the slowest diffusivity.…”