Achieving Crystal-to-Amorphous Transition without Phase Collapse in a Stable Gd-Based High-Entropy Perovskite Anode

Transition metal oxide anodes are plagued by severe volume expansion and structural collapse, which drastically shorten their cycling lifespans in lithium-ion batteries. Herein, we report an orthorhombic ABO₃-type Gd(FeCoNiCrMn)O₃ (Gd-HEO) material in which lattice-site and high-entropy engineering synergistically boost structural integrity and cycling stability. The A-site Gd builds a rigid 4f scaffold and induces tilting of the BO₆ octahedra, thereby expanding ion transport channels. Meanwhile, the mixed cations at the B-site not only promotes delocalize electrons but, more importantly, establishes a stress-dissipation network. Experimental results show that entropy-driven structural disorder triggers a self-limiting crystal-to-amorphous transition. Specifically, the material fragments into ∼2 nm nanodomains embedded in an amorphous matrix, forming a semicohesive nanoarchitecture that absorbs volume-change stress through structural adjustment. Benefiting from these structural merits, the Gd-HEO electrode retains 88% capacity after 1000 cycles with minimal volume variation, underscoring elemental diversity as a key to optimizing multication electrode materials.