ABSTRACT Rechargeable aluminum batteries (RABs) with organic cathodes emerge as promising candidates for large‐scale energy storage due to the abundant reserves, eco‐friendliness, and low costs. However, the large active ions (AlCl 2 (urea) 2 + , AlCl 4 − ) usually cause high steric hindrance in traditional cathodes with limited capacity and kinetics. Herein, to enable the efficient storage and transport of large active ions, an “in‐plane locking” strategy is first proposed to target adjusting atomic‐level steric hindrance, achieving high‐performance RABs. The “in‐plane locking” engineering drastically enhances active site utilization (over 25% promotion) toward large‐sized active ions with low steric hindrance, achieving one of the highest practical capacities of 249.4 mAh g −1 at 0.1 A g −1 . The optimized axial locking molecular engineering enables structural stability and π – π stacking, which drastically suppresses structural dissociation via interfacial stabilization, thereby delivering exceptional cycling stability (over 81.1 mAh g −1 at 1.0 A g −1 after 3500 cycles). The newly developed “in‐plane locking” cathode establishes a novel design direction for high‐performance RABs and other large‐sized active‐ion batteries systems.
Han et al. (Tue,) studied this question.