Ultrafast, Highly Reversible, and Cycle‐Stable Lithium Storage Boosted by Pseudocapacitance in Sn‐Based Alloying Anodes

Abstract Boosting power density is one of the primary challenges that current lithium ion batteries face. Alloying anodes that possess suitable potential windows stand at the forefront in pursuing ultrafast and highly reversible lithium storage to achieve high power/energy lithium ion batteries. Herein, ultrafast lithium storage in Sn‐based nanocomposite anodes is demonstrated, which is boosted by pseudocapacitance benefitting from a high fraction of highly interconnected interfaces of Fe/Sn/Li₂O. By tailoring the voltage window in the range of 0.005–1.2 V for the alloying/dealloying reactions, such Sn‐based nanocomposite anodes achieve simultaneous ultrahigh rate capability, superlong cycling performance, and close‐to‐100% Coulombic efficiency. The nanocomposite anode delivers a high reversible capacity (≈420 mAh g⁻¹) at 1 A g⁻¹ for more than 1200 cycles, corresponding to only 0.016% per cycle of capacity decay. A reversible capacity of 350 mAh g⁻¹ can be maintained at an ultrahigh current density of 80 A g⁻¹, with 67.3% capacity retention relative to the capacity at 1 A g⁻¹. This combination of pseudocapacitive lithium storage and spatially confined electrochemical reactions in Sn‐based nanocomposite anode materials may pave the way for the development of high power/energy and long life lithium ion batteries.