Enhancing Capacity Retention in Commercial Cathode Active Materials through Configurational Entropy: An Ab-Initio Simulation Study

• Published in: Meeting abstracts (Electrochemical Society) Vol. MA2025-01; no. 3; p. 417
• Main Authors: Yim, Chae-Ho, Baranova, Elena A., Abu-Lebdeh, Yaser A.
• Format: Journal Article
• Language: English
• Published: The Electrochemical Society, Inc 11.07.2025
• ISSN: 2151-2043; 2151-2035
• DOI: 10.1149/MA2025-013417mtgabs

Cathode-active materials (CAMs) play a crucial role in enhancing the energy density and reducing the cost of Li-ion battery cells. In commercially-relevant layered oxides such as LiNi x Mn y Co z O 2 (NMCs), efforts to minimize cobalt content while maximizing nickel content have led to significant improvements in energy density. However, higher nickel content has also resulted in lower capacity retention compared to first-generation NMC-CAMs with equal proportions of nickel, manganese, and cobalt (x=y=z=1) or with cobalt as the dominant component (z=1, x=y=0). To address this challenge, this study explores the high-entropy concept as a strategy to improve capacity retention without compromising energy density. We present evidence of configurational entropy effects in commercial CAMs by measuring different states of lithiation or states of charge in half-cells. These experimental results are corroborated with Ab-initio simulations, providing a comprehensive understanding of the configurational entropy effect and guiding the design of next-generation CAMs.