ABSTRACT Coordinatively unsaturated single‐atom nanozymes with sufficient H 2 O 2 adsorption and rapid kinetics display excellent peroxidase (POD)‐like activity; however, their rational construction limits their wide application for cancer therapy. Here, we report a ligand chelation‐determined conformation (LCDC) strategy to construct Cu single‐atom nanozymes supported on carbon dots (Cu‐N 2 ‐CDs) that were realized by in situ chelation and carbonization of organic chelating agent and metal cation. Such coordinatively unsaturated Cu‐N 2 ‐CDs expose high‐spin Cu sites that enhance d‐p orbital hybridization to facilitate H 2 O 2 adsorption. Importantly, the coordinatively unsaturated Cu‐N 2 configuration is capable of elevating the electron density at the metal center and narrowing the band gap to accelerate •OH generation reaction kinetics. The Cu‐N 2 ‐CDs outperform their Cu‐N 4 counterparts by achieving a 3.49‐fold stronger H 2 O 2 adsorption and a 3.62‐fold greater maximum reaction rate, leading to the efficient production of toxic •OH from endogenous H 2 O 2 . Consequently, Cu‐N 2 ‐CDs achieve excellent tumor catalytic therapy outcomes both in vitro and in vivo. This work provides fundamental insights for the rational design of high‐performance nanozymes through precise coordination engineering.
Lin et al. (Wed,) studied this question.
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