Design of Gradient Ti Reconstituted Fe2O3 Anodes with Enhanced Lithium Affinity Modulated Electronic Structures: First-Principles Calculations and Experiment Verification

High-performance conversion transition metal oxides are strong candidates for advanced anode materials for lithium-ion batteries. However, the poor intrinsic conductivity and the large volume changes during battery operation are important constraints to its practical application. The heterogeneous atom doping strategy is an important way to modulate the electronic structure and surface states of the host materials. Herein, theoretical calculations reveal that heteroatomic Ti doping and its ionic or electronic compensation mechanisms can well modulate the electronic structure of Fe2O3 and change the surface Li-ion affinity. A Ti concentration gradient modification strategy for Fe2O3 is proposed to construct high-performance electrode materials. As a Li-ion battery anode, Ti concentration gradient-doped Fe2O3 achieves excellent long-cycle stability, with a reversible capacity of 1001.9 mAh g–1 at 1 A g–1 for 1200 cycles, and even maintains a reversible specific capacity compared to the theoretical capacity of commercial graphite electrodes at 2 A g–1 for 2000 cycles. This combination of theoretical calculations and experiments offers ways to intelligently design and develop alkali metal ion batteries.