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This study proposed a new layer modification technique, “layer charge control”, for layered perovskites, and the structures of the obtained charge neutral [CeTa 2 O 7 ] perovskite sheet were characterized theoretically and experimentally.

Ce(iv)-centered charge-neutral perovskite layers topochemically derived from anionic [CeTa2O7]−layers

Ce(iv)-centered charge-neutral perovskite layers topochemically derived from anionic [CeTa₂O₇]⁻layers