Work

Origin of Electrochemical Activation Leading to Enhanced Cycling Stability of Li‐ and Mn‐Rich Cathodes

Year: 2026

Type: article

Abstract: ABSTRACT Electrochemical activation is a critical step for optimal functioning of Li‐ and Mn‐rich (LMR) cathodes, yet the underlying mechanism for such activation remains elusive. Here, by using scanning/transmission electron microscopy (S/TEM) combined with the associated energy‐dispersive x‐ray spectroscopy (EDS) and electron energy‐loss spectroscopy (EELS), we decipher the origin of the activation enhanced electrochemical properties. We reveal that activation induces the formation of a spinel‐like phase within the C2/m domains of the LMR cathode, where the transition‐metal ions partially occupy both the tetrahedral (8a) and octahedral (16c) sites of the Fd m spinel lattice, distinguishing the spinel‐like phase from the conventional high‐voltage spinel. Systematic varying the cycling voltage reveals a critical activation voltage above which this spinel‐like phase forms, while lower voltages preserve the layered bulk structure. As the spinel‐like phase is a stable structure for electrochemical cycling, the present findings provide direct mechanistic insight into the voltage‐dependent activation process and explain how the C2/m to spinel‐like transformation upon activation contributes to the electrochemical performance of LMR cathodes, providing guidance for the rational design of Li‐rich cathodes with enhanced cycling durability.

Source: Angewandte Chemie

DOI: 10.1002/ange.8818196

Authors: Peng Zuo, Daniel P. Abraham, Chongmin Wang

Institutions: Pacific Northwest National Laboratory, Environmental Molecular Sciences Laboratory, Argonne National Laboratory

Language: English

Topic: Advancements in Battery Materials

Subfield: Electrical and Electronic Engineering

Field: Engineering

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: hybrid

Estimated APC paid: $5,790