Localized Ligands Assist Ultrafast Multivalent‐Cation Intercalation Pseudocapacitance

Rechargeable batteries based on multivalent cation (Mvn+, n>1) carriers are considered potentially low-cost alternatives to lithium-ion batteries. However, the high charge-density Mvn+ carriers generally lead to sluggish kinetics and poor structural stability in cathode materials. Herein, we report an Mvn+ storage via intercalation pseudocapacitance mechanism in a 2D bivalve-like organic framework with localized ligands. By switching from conventional intercalation to localized ligand assisted-intercalation pseudocapacitance, the organic cathode exhibits unprecedented fast kinetics with little structural change upon intercalation. It thus enables an excellent power density of 57 kW/kg over 20000 cycles for Ca2+ storage and a power density of 14 kW/kg with a long cycling life over 45000 cycles for Zn2+ storage. This work may provide a largely unexploited route toward constructing a local dynamic coordination microstructure for ultrafast Mvn+ storage.