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      One‐Dimensional Covalent Organic Framework as High‐Performance Cathode Materials for Lithium‐Ion Batteries

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          Abstract

          Covalent organic frameworks (COFs) have emerged as a new class of cathode materials for energy storage in recent years. However, they are limited to two‐dimensional (2D) or three‐dimensional (3D) framework structures. Herein, this work reports designed synthesis of a redox‐active one‐dimensional (1D) COF and its composites with 1D carbon nanotubes (CNTs) via in situ growth. Used as cathode materials for Li‐ion batteries, the 1D COF@CNT composites with unique dendritic core–shell structure can provide abundant and easily accessible redox‐active sites, which contribute to improve diffusion rate of lithium ions and the corresponding specific capacity. This synergistic structural design enables excellent electrochemical performance of the cathodes, giving rise to 95% utilization of redox‐active sites, high rate capability (81% capacity retention at 10 C), and long cycling stability (86% retention after 600 cycles at 5 C). As the first example to explore the application of 1D COFs in the field of energy storage, this study demonstrates the great potential of this novel type of linear crystalline porous polymers in battery technologies.

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          Li-ion battery materials: present and future

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            30 Years of Lithium-Ion Batteries

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              High-rate electrochemical energy storage through Li+ intercalation pseudocapacitance.

              Pseudocapacitance is commonly associated with surface or near-surface reversible redox reactions, as observed with RuO2·xH2O in an acidic electrolyte. However, we recently demonstrated that a pseudocapacitive mechanism occurs when lithium ions are inserted into mesoporous and nanocrystal films of orthorhombic Nb2O5 (T-Nb2O5; refs 1,2). Here, we quantify the kinetics of charge storage in T-Nb2O5: currents that vary inversely with time, charge-storage capacity that is mostly independent of rate, and redox peaks that exhibit small voltage offsets even at high rates. We also define the structural characteristics necessary for this process, termed intercalation pseudocapacitance, which are a crystalline network that offers two-dimensional transport pathways and little structural change on intercalation. The principal benefit realized from intercalation pseudocapacitance is that high levels of charge storage are achieved within short periods of time because there are no limitations from solid-state diffusion. Thick electrodes (up to 40 μm thick) prepared with T-Nb2O5 offer the promise of exploiting intercalation pseudocapacitance to obtain high-rate charge-storage devices.
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                Author and article information

                Contributors
                Journal
                Small
                Small
                Wiley
                1613-6810
                1613-6829
                June 2023
                March 14 2023
                June 2023
                : 19
                : 24
                Affiliations
                [1 ] Key Laboratory of Synthetic and Self‐Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences 345 Lingling Road Shanghai 200032 China
                Article
                10.1002/smll.202300518
                f5ccee59-6d3a-4183-8c3b-37c11a56bca9
                © 2023

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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