Regulating segmental dynamics for ion clusters in polymer binders to realize high-areal-capacity electrodes in lithium batteries

Abstract

The growing demand for high-energy-density lithium batteries necessitates high-areal-capacity electrodes, typically involving high-mass-loading cathodes. However, achieving high mass-loading cathodes often leads to challenges such as structural instability and inefficient ion transport. In this study, a series of ionic soft polymer (ISP) binders have been designed to overcome these limitations. By modulating the segmental dynamics in the side chains, the ISP binder forms a reversible ion cluster, significantly enhancing ionic conductivity. Furthermore, electrostatic interactions and hydrogen bonding within the binder foster a robust network, providing strong adhesion and stability, while minimizing transition metal dissolution and surface side reactions. The ISP binder also exhibits remarkable self-healing properties and stretchability, effectively accommodating solvent-drying-induced stress. The designed binder-incorporated NCM811 cathodes achieve an impressive areal capacity of 17.9 mA h cm−2 at 86.1 mg cm−2 mass loading. A pouch-type Li metal full cell with a thin Li metal anode (40 μm) delivers a high energy density of 381.1 W h kgcell−1/1067.5 W h Lcell−1, including packaging materials. This study demonstrates the promising potential of ISP binder to enable scalable high-areal-capacity electrodes for high-energy-density lithium batteries with enhanced stability and performance.

Graphical abstract: Regulating segmental dynamics for ion clusters in polymer binders to realize high-areal-capacity electrodes in lithium batteries

Supplementary files

Article information

Article type
Paper
Submitted
31 Mar 2025
Accepted
06 Jun 2025
First published
27 Jun 2025
This article is Open Access
Creative Commons BY-NC license

Energy Environ. Sci., 2025, Advance Article

Regulating segmental dynamics for ion clusters in polymer binders to realize high-areal-capacity electrodes in lithium batteries

D. Han, S. Kim, Y. Kim, H. Lim, G. R. Lee, C. K. Song, W. Song, H. C. Moon, S. Park and T. Park, Energy Environ. Sci., 2025, Advance Article , DOI: 10.1039/D5EE01785H

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