Abstract
Pursuing nanozymes with predominant catalytic activities holds great potential in meeting the needs of multi-field applications, such as in the environment, yet remains challenging. Herein, the cutting-edge strategies for boosting nanozyme catalysis are systematically analyzed from four synergistic dimensions, and a theoretical framework is developed integrating morphological structure, electronic structure, external stimulation, and machine learning (ML)-aided design. From the morphological perspective, the structure-activity relationship between nanostructures and catalytic performance is elucidated, revealing the regulatory mechanism underlying active site exposure, substrate accessibility, and electron transfer kinetics. Subsequently, the electronic structure governed by catalytic activities through precisely optimizing adsorption energy and reaction pathways, such as d-band center, e(g) occupancy, defect engineering, spin state, etc., is discussed in depth. Then, the mechanism underlying the dynamic regulation of catalytic activity via external stimulations, such as ultrasound, light, electric field, etc., is systematically summarized. Notably, the revolutionary role of ML-driven high-throughput screening in analyzing complex structure-activity relationships and accelerating the discovery of high-performance nanozymes is emphasized. Ultimately, this paper highlights the key role of interdisciplinary integration, encompassing material science, catalytic engineering, and artificial intelligence, etc., in overcoming current bottlenecks, unlocking the potential of nanozymes to address global challenges, and providing a new perspective for advancing the development of nanozymology.