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Ultrathin positively charged electrode skin for durable anion-intercalation battery chemistries

Sabaghi, D.; Wang, Z.; Bhauriyal, P.; Lu, Q.; Morag, A.; Mikhailovia, D.; Hashemi, P.; Li, D.; Neumann, C.; Liao, Z.; Dominic, A. M.; Nia, A. S.; Dong, R.; Zschech, E.; Turchanin, A.; Heine, T.; Yu, M.; Feng, X.

Abstract

The anion-intercalation chemistries of graphite have the potential to construct batteries with promising energy and power breakthroughs. Here, we report the use of an ultrathin, positively charged two-dimensional poly(pyridinium salt) membrane (C2DP) as the graphite electrode skin to overcome the critical durability problem. Large-area C2DP enables the conformal coating on the graphite electrode, remarkably alleviating the electrolyte. Meanwhile, the dense face-on oriented single crystals with ultrathin thickness and cationic backbones allow C2DP with high anion-transport capability and selectivity. Such desirable anion-transport properties of C2DP prevent the cation/solvent co-intercalation into the graphite electrode and suppress the consequent structure collapse. An impressive PF6−-intercalation durability is demonstrated for the C2DP-covered graphite electrode, with capacity retention of 92.8% after 1000 cycles at 1 C and Coulombic efficiencies of > 99%. The feasibility of constructing artificial ion-regulating electrode skins with precisely customized two-dimensional polymers offers viable means to promote problematic battery chemistries.

Keywords: batteries; dft; 2d polymers

Permalink: https://www.hzdr.de/publications/Publ-36899