Tuning the Electronic Configuration of Oxygen Atom in Engineering Non‐Self‐Limited Nanozyme for Portable Immunosensor

Abstract Nanozymes are conceived to replace natural enzymes to avoid expensive processing techniques and fragile reservation conditions. Unfortunately, the self‐limited reaction has run counter to the desire for sustainable catalysis as natural enzymes. Herein, the universal mechanism to overcome the self‐limitation of nanozymes caused by the absorption of ions on the active sites is explored. Therefore, the dual noble metals (Au/Pt) are introduced as the center to synthesize two kinds of nanozymes with different types of central metal elements (Cu and Ce) and also compounds (metal‐organic framework and metallic oxide), showing a similar bond between a central metal and oxygen atom. The morphology characterization and density functional theory calculations demonstrate that the improvement in the electronic environment of neighboring oxygen atoms by inducing the charge redistribution via the bond between noble metals and compounds is crucial for enhancing catalytic activity and avoiding the adsorption of the nontarget substrate. This work not only experimentally proves that the adjustment on the electronic environment of adjacent atoms in the catalytic center is a feasible and universal approach to overcome the self‐limited reaction, but also achieves the application of self‐powered and portable immunosensor to broaden nanozymes in sensitive detection of illegal addition in food.