Zn2+-Imidazole Coordination Crosslinks for Elastic Polymeric Binders in High-Capacity Silicon Electrodes

Jaemin Kim; Kiho Park; Yunshik Cho; Hyuksoo Shin; Sungchan Kim; Kookheon Char; Jang Wook Choi

doi:10.1002/advs.202004290

Zn²⁺-Imidazole Coordination Crosslinks for Elastic Polymeric Binders in High-Capacity Silicon Electrodes

Adv Sci (Weinh). 2021 Mar 2;8(9):2004290. doi: 10.1002/advs.202004290. eCollection 2021 May.

Authors

Jaemin Kim¹, Kiho Park¹, Yunshik Cho¹, Hyuksoo Shin¹, Sungchan Kim¹, Kookheon Char¹, Jang Wook Choi^{1

2}

Affiliations

¹ School of Chemical and Biological Engineering and Institute of Chemical Process Seoul National University 1 Gwanak-ro, Gwanak-gu Seoul 08826 Republic of Korea.
² Department of Materials Science and Engineering Seoul National University 1 Gwanak-ro, Gwanak-gu Seoul 08826 Republic of Korea.

Abstract

Recent research has built a consensus that the binder plays a key role in the performance of high-capacity silicon anodes in lithium-ion batteries. These anodes necessitate the use of a binder to maintain the electrode integrity during the immense volume change of silicon during cycling. Here, Zn²⁺-imidazole coordination crosslinks that are formed to carboxymethyl cellulose backbones in situ during electrode fabrication are reported. The recoverable nature of Zn²⁺-imidazole coordination bonds and the flexibility of the poly(ethylene glycol) chains are jointly responsible for the high elasticity of the binder network. The high elasticity tightens interparticle contacts and sustains the electrode integrity, both of which are beneficial for long-term cyclability. These electrodes, with their commercial levels of areal capacities, exhibit superior cycle life in full-cells paired with LiNi_0.8Co_0.15Al_0.05O₂ cathodes. The present study underlines the importance of highly reversible metal ion-ligand coordination chemistries for binders intended for high capacity alloying-based electrodes.

Keywords: carboxymethyl cellulose; dynamic crosslinking; elastic binders; in situ crosslinking; metal–ligand coordination; silicon/carbon composite; supramolecular chemistry.