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NiFe-LDHs have been deemed as a benchmark non-noble metal electrocatalysts for oxygen evolution reaction (OER). However, for NiFe-LDHs laminate, the edge sites are active, but the basal plane is inert, leading to underutilization for the OER catalysts. Herein, it is the first time to intercalate the light and electron-deficient Li ion into NiFe-LDHs basal plane. The results of theoretical calculation and experiment both showed that the electron would transfer from near Ni 2+ to the surrounding of Li + , resulting in the electron-deficient