Title of the paper: Localized Ligands Assist Ultrafast Multivalent-Cation Intercalation Pseudocapacitance
First author: Luting Xie (Huaqiao University)
Co-First author: Kui Xu (Nanjing Tech University)
Corresponding authors: Hongwei Chen (Huaqiao University), Guan Wu (Zhejiang Sci-Tech University)
Compared to traditional monovalent cation storage (M⁺, including Li⁺, Na⁺, K⁺, etc.), the storage of multivalent metal ions (Mv^(n+), n>1) involves multi-step electron transfer and can serve as charge carriers to build safer, cheaper, and higher-energy multivalent ion batteries. However, traditional electrode materials for storing Mv^(n+) generally need to meet multiple conditions simultaneously, including having a material framework with multi-electron redox centers and matching the coordination environment of Mv^(n+) with the active sites of the framework. Even if the electrode material meets the above conditions, the high charge density of Mv^(n+) limits its electrode kinetics. Moreover, the storage process of high charge density Mv^(n+) is often accompanied by irreversible phase changes in the electrode material, thus limiting the long cycle life of the electrode. Therefore, overcoming the limitations of traditional Mv^(n+) storage modes and achieving fast kinetics and long-life Mv^(n+) storage is a major challenge in the field of electrochemical energy storage.
Based on this, the team of Hongwei Chen from Huaqiao University and the team of Guan Wu from Zhejiang Sci-Tech University, among others, designed a type of organic framework cathode material for Mv^(n+) storage based on the intercalation pseudocapacitance mechanism. The basic mechanism is that the Mv^(n+) entering the framework can be shielded by localized anionic ligands, thus being stably stored near the surface of the framework material. This localized ligand promotes ultrafast intercalation capacitance behavior of multivalent metal ions in the organic framework, thus achieving fast and stable storage of Zn²⁺ and Ca²⁺. This organic framework material achieved reversible storage of Zn²⁺ for over 45,000 cycles and Ca²⁺ for over 20,000 cycles, with power densities reaching 14 and 57 kW/kg, respectively, and demonstrated stable long-cycle performance and excellent kinetic performance. This work was published in the international top journal Angewandte Chemie, with Luting Xie and Kui Xu as the co-first authors.
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