4.8 Article

Bilayered Ca0.28V2O5?H2O: High-Capacity Cathode Material for Rechargeable Ca-Ion Batteries and Its Charge Storage Mechanism

Journal

CHEMISTRY OF MATERIALS
Volume 34, Issue 4, Pages 1491-1498

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c02774

Keywords

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Funding

  1. National Research Foundation of Korea (NRF) - Korea government (MSIT) [2020R1A2C2007070, 2020R1A4A4079810]
  2. National Research Foundation of Korea [2020R1A2C2007070] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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This study reports a bilayered Ca0.28V2O5·H2O as a high-capacity CIB cathode material with excellent capacity and cyclability. Its unique intercalation mechanism and highly reversible charge-discharge cycle provide valuable insights for developing high-performance CIB cathodes.
Despite the attractive theoretical benefits of calcium-ion batteries (CIBs) as post-lithium-ion batteries, only a limited number of host materials are known to reversibly intercalate calcium ions to date, and their intercalation mechanism is barely understood. Herein, we report bilayered Ca0.28V2O5middotH2O as a highcapacity CIB cathode material. It exhibits a capacity of 142 mA h g-1 at similar to 3.0 V vs Ca/Ca2+ and excellent cyclability. Ca0.28V2O5middotH2O undergoes irreversible structural transformation to a two-fold superstructure during the first charge, which triggers its electrochemical activity from the subsequent cycling. Its intercalation mechanism is unique; upon charging, complete calcium extraction occurs from every two interlayers, maintaining only a fraction of calcium ions in the other interlayers; on discharge, calcium ions are irregularly inserted into the interlayers, resulting in stacking faults. This charge-discharge cycle is highly reversible. This work would be the first report that experimentally unveils the electrochemical calcium storage mechanism of an intercalation host material, providing valuable insights for developing high-performance CIB cathodes.

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