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 repo...

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Bibliographic Details
Published in:Angewandte Chemie 2023-06, Vol.135 (26), p.n/a
Main Authors: Xie, Luting, Xu, Kui, Sun, Wenlu, Fan, Yingzhu, Zhang, Junyu, Zhang, Yixiao, Zhang, Hui, Chen, Jun, Shen, Yanbin, Fu, Fang, Kong, Huabin, Wu, Guan, Wu, Jihuai, Chen, Liwei, Chen, Hongwei
Format: Article
Language:English
Subjects:
Batteries
Calcium ions
Carrier density
Cathodes
Cations
Chemistry
Current carriers
Electrode materials
Intercalation
Intercalation Pseudocapacitance
Kinetics
Ligands
Lithium
Lithium-ion batteries
Mollusks
Multivalent Ion Batteries
Organic Frameworks
Rechargeable batteries
Stability
Structural stability
Zinc
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Summary: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 featured 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−1 over 20000 cycles for Ca2+ storage and a power density of 14 kW kg−1 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. By switching from conventional intercalation to localized ligand‐assisted‐intercalation pseudocapacitance, the organic cathode exhibits unprecedented fast kinetics with little structural change upon ion intercalation.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202300372