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.