Ultrahigh Capacity from Complexation-Enabled Aluminum-Ion Batteries with C<sub>70</sub> as the Cathode.
basic_science · Level V
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- Record sourced from PubMed, PMID 37815787.
- Also identified by DOI 10.1002/adma.202306244.
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Abstract
Restricted by the available energy storage modes, currently rechargeable aluminum-ion batteries (RABs) can only provide a very limited experimental capacity, regardless of the very high gravimetric capacity of Al (2980 mAh g<sup>-1</sup> ). Here, a novel complexation mechanism is reported for energy storage in RABs by utilizing 0D fullerene C<sub>70</sub> as the cathode. This mechanism enables remarkable discharge voltage (≈1.65 V) and especially a record-high reversible specific capacity (750 mAh g<sup>-1</sup> at 200 mA g<sup>-1</sup> ) of RABs. By means of in situ Raman monitoring, mass spectrometry, and density functional theory (DFT) calculations, it is found that this elevated capacity is attributed to the direct complexation of one C<sub>70</sub> molecule with 23.5 (super)halogen moieties (superhalogen AlCl<sub>4</sub> and/or halogen Cl) in average, forming (super)halogenated C<sub>70</sub> ·(AlCl<sub>4</sub> )<sub>m</sub> Cl<sub>n-m</sub> complexes. Upon discharging, decomplexation of C<sub>70</sub> ·(AlCl<sub>4</sub> )<sub>m</sub> Cl<sub>n-m</sub> releases AlCl<sub>4</sub> <sup>-</sup> /Cl<sup>-</sup> ions while preserving the intact fullerene cage. This work provides a new route to realize high-capacity and long-life batteries following the complexation mechanism.