Regulating the H₂O₂ Activation Pathway on a Well-Defined CeO₂ Nanozyme Allows the Entire Steering of Its Specificity between Associated Enzymatic Reactions

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Abstract

Nanozymes are promising alternatives to natural enzymes, but their use remains limited owing to poor specificity. For example, CeO₂ activates H₂O₂ and displays peroxidase (POD)-like, catalase (CAT)-like, and haloperoxidase (HPO)-like activities. Since they unavoidably compete for H₂O₂, affecting its utilization in the target application, the precise manipulation of reaction specificity is thus imperative. Herein, we showed that one can simply achieve this by manipulating the H₂O₂ activation pathway on pristine CeO₂ in well-defined shapes. This is because the coordination and electronic structures of Ce sites vary with CeO₂ surfaces, wherein the (100) and (111) surfaces display nearly 100% specificity toward POD-/CAT-like and HPO-like activities, respectively. The antibacterial results suggest that the latter surface can well-utilize H₂O₂ to kill bacteria (cf., the former), which is promising for anti-biofouling applications. This work provides atomic insights into the synthesis of nanozymes with improved activity, reaction specificity, and H₂O₂ utilization.

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