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Modulating non-electrochemical (de)intercalation processes in layered vanadium oxides for enhanced calcium-ion storage
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DOI：10.1007/s11426-026-3586-7.png)
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Abstract
En 中文
Calcium-ion batteries (CIBs) are promising candidates for post-lithium-ion batteries but face challenges including unsuitable cathodes and unclear failure mechanisms. Herein, a reconstructed vanadium oxide (Li@MgVO) is employed to investigate interlayer ion evolution during Ca2+-storage. Experiments and theory reveal that the previously overlooked non-electrochemical (de)intercalation processes of interlayer ions critically impact Ca2+-storage. Specifically, although Ca2+ can intercalate into host materials without an applied electrochemical driving force, they do not contribute to the discharge capacity and, more seriously, hinders complete Ca2+ deintercalation. Encouragingly, pre-intercalated Mg2+ and Li+ in Li@MgVO interlayers can exchange with Ca2+ during cycling, and this “pre-intercalation-exchange” mechanism effectively minimizes the undesirable Ca2+ intercalated via non-electrochemical processes. Consequently, the assembled Ca-ion hybrid capacitor exhibits a high capacity of 60 mAh g−1 at 500 mA g−1 with a capacity retention of 97.13% after 300 cycles, significantly higher than that of unmodified vanadium oxide (18 mAh g−1 and 80.45% capacity retention).
Keywords:
calcium-ion battery
layered vanadium oxides
Ca2+-storage mechanism
non-electrochemical processes
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