Chemomechanical damage prediction from phase-field simulation video sequences using a deep-learning-based methodology.

Understanding the failure mechanisms of lithium-ion batteries is essential for their greater adoption in diverse formats. Operando X-ray and electron microscopy enable the evaluation of concentration, phase, and stress heterogeneities in electrode architectures. Phase-field models are commonly used to capture multi-physics coupling including the interplay between electrochemistry and mechanics.

Chemistry-mechanics-geometry coupling in positive electrode materials: a scale-bridging perspective for mitigating degradation in lithium-ion batteries through materials design.

Despite their rapid emergence as the dominant paradigm for electrochemical energy storage, the full promise of lithium-ion batteries is yet to be fully realized, partly because of challenges in adequately resolving common degradation mechanisms. Positive electrodes of Li-ion batteries store ions in interstitial sites based on redox reactions throughout their interior volume. However, variations in the local concentration of inserted Li-ions and inhomogeneous intercalation-induced structural transformations beget substantial stress.

Cation reordering instead of phase transitions: Origins and implications of contrasting lithiation mechanisms in 1D ζ- and 2D α-VO.

Substantial improvements in cycle life, rate performance, accessible voltage, and reversible capacity are required to realize the promise of Li-ion batteries in full measure. Here, we have examined insertion electrodes of the same composition (VO) prepared according to the same electrode specifications and comprising particles with similar dimensions and geometries that differ only in terms of their atomic connectivity and crystal structure, specifically two-dimensional (2D) layered α-VO that crystallizes in an orthorhombic space group and one-dimensional (1D) tunnel-structured ζ-VO crystallized in a monoclinic space group. By using particles of similar dimensions, we have disentangled the role of specific structural motifs and atomistic diffusion pathways in affecting electrochemical performance by mapping the dynamical evolution of lithiation-induced structural modifications using ex situ scanning transmission X-ray microscopy, synchrotron X-ray diffraction measurements, and phase-field modeling.

Effect of crystallite geometries on electrochemical performance of porous intercalation electrodes by multiscale operando investigation.

Lithium-ion batteries are yet to realize their full promise because of challenges in the design and construction of electrode architectures that allow for their entire interior volumes to be reversibly accessible for ion storage. Electrodes constructed from the same material and with the same specifications, which differ only in terms of dimensions and geometries of the constituent particles, can show surprising differences in polarization, stress accumulation and capacity fade. Here, using operando synchrotron X-ray diffraction and energy dispersive X-ray diffraction (EDXRD), we probe the mechanistic origins of the remarkable particle geometry-dependent modification of lithiation-induced phase transformations in VO as a model phase-transforming cathode.