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Layer-structured birnessite (d-MnO 2 ) has been applied recently in the heterogeneous Fenton-like process. However, easy deactivation and low utilization efficiency of H 2 O 2 limit its practical application. The catalytic processes of H 2 O 2 on birnessite were successfully regulated via surface chemical modification as Cu 2 + ions were intercalated into the birnessite by the ion-exchange method (CuBir). The triple-corner-sharing inner-sphere surface complexes of Cu 2 + ions (TCS species) formed above Mn vacancies could effectively weaken the over-complexation of H 2 O 2 on the surface of [MnO 6 ] sheets, and then decrease the self-consumption of surface-formed superoxide radicals. The surface TCS species have excellent Fenton-like performances and enhance the conversion efficiency of H 2 O 2 into reactive oxygen species (ROS). Moreover, the surface Cu 2 + -modification engineering could prevent deactivation owing to degradation intermediate residues and improve the recyclability of catalyst.

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