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The two-dimensional (2D) materials with asymmetric sub-layers have recently attracted tremendous interest in many fields, and investigating the structure-performance relationship of different sub-layers is critical but challenging. Herein, we report that natural kaolinite (Kaol) nanosheets with an asymmetric layer structure possess a contrasting photocatalytic activity on its Al-O and Si-O sub-layers. The experimental and theoretical results reveal that the ion isovalent structure of Fe3+ and Al3+ not only results in a high iron doping c
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