Single-Crystal α-Fe₂O₃ with Engineered Exposed (001) Facet for High-Rate, Long-Cycle-Life Lithium-Ion Battery Anode

Designing electrode materials with engineered exposed facets provides a novel strategy to improve their electrochemical properties. However, the controllability of the exposed facet remains a daunting challenge, and a deep understanding of the correlation between exposed facet and Li⁺-transfer behavior has been rarely reported. In this work, single-crystal α-Fe₂O₃ hexagonal nanosheets with an exposed (001) facet are prepared with the assistance of aluminum ions through a one-step hydrothermal process, and structural characterizations reveal an Al³⁺-concentration-dependent-growth mechanism for the α-Fe₂O₃ nanosheets. Furthermore, such α-Fe₂O₃ nanosheets, when used as lithium-ion battery anodes, exhibit high specific capacity (1261.3 mAh g^-1 at 200 mA g^-1), high rate capability (with a reversible capacity of approximately 605 mAh g^-1 at 10 A g^-1), and excellent cyclic stability (with a capacity of over 900 mAh g^-1 during 500 cycles). The superior electrochemical performance of α-Fe₂O₃ nanosheets is attributed to the pseudocapacitive behavior, Al-doping in the α-Fe₂O₃ structure, and improved Li⁺-transfer property across the (001) facet, as elucidated by first-principles calculations based on density functional theory. These results reveal the underlying mechanism of Li⁺ transfer across different facets and thus provide insights into the understanding of the excellent electrochemical performance.