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Localized Ligands Assist Ultrafast Multivalent-Cation Intercalation Pseudocapacitance
Authors:Luting Xie  Prof. Kui Xu  Wenlu Sun  Yingzhu Fan  Dr. Junyu Zhang  Dr. Yixiao Zhang  Dr. Hui Zhang  Jun Chen  Prof. Yanbin Shen  Prof. Fang Fu  Dr. Huabin Kong  Prof. Guan Wu  Prof. Jihuai Wu  Prof. Liwei Chen  Prof. Hongwei Chen
Affiliation:1. College of Materials Science and Engineering, Huaqiao University, Xiamen, 361021 China

These authors contributed equally to this work.;2. School of Flexible Electronics (Future Technologies) & Institute of Advanced Materials (IAM), Nanjing University of Technology, Nanjing, 211816 China

These authors contributed equally to this work.;3. College of Materials Science and Engineering, Huaqiao University, Xiamen, 361021 China;4. i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123 Jiangsu Province, China;5. Instrumental Analysis Center, Laboratory and Equipment Management Department, Huaqiao University, Xiamen, Fujian, 361021 China;6. In-Situ Center for Physical Science, School of Chemistry and Chemical Engineering, Shanghai Jiaotong University, Shanghai, 200240 China;7. National Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University, Yinchuan, 750021 China;8. National Engineering Lab for Textile Fiber Materials and Processing Technology, School of Materials Science and Engineering, Zhejiang Sci-Tech University, Hangzhou, 310018 China

Abstract: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.
Keywords:Cathodes  Intercalation Pseudocapacitance  Multivalent Ion Batteries  Organic Frameworks  Stability
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