Nowadays, research on electrochemical storage systems moves into the direction of post-lithium-ion batteries, such as aluminum-ion batteries, and the exploration of suitable materials for such batteries. Vanadium pentoxide (V2
) is one of the most promising host materials for the intercalation of multivalent ions. Here, we report on the fabrication of a binder-free and self-supporting V2
micrometer-thick paper-like electrode material and its use as the cathode for rechargeable aluminum-ion batteries. The electrical conductivity of the cathode was significantly improved by a novel in-situ and self-limiting copper migration approach into the V2
structure. This process takes advantage of the dissolution of Cu by the ionic liquid-based electrolyte, as well as the presence of two different accommodation sites in the nanostructured V2
available for aluminum-ions and the migrated Cu. Furthermore, the advanced nanostructured cathode delivered a specific discharge capacity of up to ~170 mAh g−1
and the reversible intercalation of Al3+
for more than 500 cycles with a high Coulomb efficiency reaching nearly 100%. The binder-free concept results in an energy density of 74 Wh kg−1
, which shows improved energy density in comparison to the so far published V2
-based cathodes. Our results provide valuable insights for the future design and development of novel binder-free and self-supporting electrodes for rechargeable multivalent metal-ion batteries associating a high energy density, cycling stability, safety and low cost.
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