Regulating electrostatic phenomena by cationic polymer binder for scalable high-areal-capacity Li battery electrodes

Jung-Hui Kim, Kyung Min Lee, Ji Won Kim, Seong Hyeon Kweon, Hyun-Seok Moon, Taeeun Yim (), Sang Kyu Kwak () and Sang-Young Lee ()
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Jung-Hui Kim: Yonsei University
Kyung Min Lee: Ulsan National Institute of Science and Technology (UNIST)
Ji Won Kim: Incheon National University
Seong Hyeon Kweon: Ulsan National Institute of Science and Technology (UNIST)
Hyun-Seok Moon: Yonsei University
Taeeun Yim: Incheon National University
Sang Kyu Kwak: Korea University
Sang-Young Lee: Yonsei University

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Despite the enormous interest in high-areal-capacity Li battery electrodes, their structural instability and nonuniform charge transfer have plagued practical application. Herein, we present a cationic semi-interpenetrating polymer network (c-IPN) binder strategy, with a focus on the regulation of electrostatic phenomena in electrodes. Compared to conventional neutral linear binders, the c-IPN suppresses solvent-drying-induced crack evolution of electrodes and improves the dispersion state of electrode components owing to its surface charge-driven electrostatic repulsion and mechanical toughness. The c-IPN immobilizes anions of liquid electrolytes inside the electrodes via electrostatic attraction, thereby facilitating Li+ conduction and forming stable cathode–electrolyte interphases. Consequently, the c-IPN enables high-areal-capacity (up to 20 mAh cm–2) cathodes with decent cyclability (capacity retention after 100 cycles = 82%) using commercial slurry-cast electrode fabrication, while fully utilizing the theoretical specific capacity of LiNi0.8Co0.1Mn0.1O2. Further, coupling of the c-IPN cathodes with Li-metal anodes yields double-stacked pouch-type cells with high energy content at 25 °C (376 Wh kgcell−1/1043 Wh Lcell–1, estimated including packaging substances), demonstrating practical viability of the c-IPN binder for scalable high-areal-capacity electrodes.

Date: 2023
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DOI: 10.1038/s41467-023-41513-1

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