Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 23, Pages 8855-8865Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c03510
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Funding
- National Natural Science Foundation of China [21721003, 21635007]
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This study demonstrates the development of a simple yet efficient redox nanozyme through defect engineering, which enhances binding capacity and catalytic activity, leading to substantial disruption of redox and metabolism homeostasis in the tumor region.
Perusing redox nanozymes capable of disrupting cellular homeostasis offers new opportunities to develop cancer-specific therapy, but remains challenging, because most artificial enzymes lack enzyme-like scale and configuration. Herein, for the first time, we leverage a defect engineering strategy to develop a simple yet efficient redox nanozyme by constructing enzyme-mimicking active centers and investigated its formation and catalysis mechanism thoroughly. Specifically, the partial Fe doping in MoOx (donated as Fe-MoOv) was demonstrated to activate structure reconstruction with abundant defect site generation, including Fe substitution and oxygen vacancy (OV) defects, which significantly enable the binding capacity and catalytic activity of Fe-MoOv nanozymes in a synergetic fashion. More intriguingly, plenty of delocalized electrons appear due to Fe-facilitated band structure reconstruction, directly contributing to the remarkable surface plasmon resonance effect in the near-infrared (NIR) region. Under NIR-II laser irradiation, the designed Fe-MoOv nanozymes are able to induce substantial disruption of redox and metabolism homeostasis in the tumor region via enzyme-mimicking cascade reactions, thus significantly augmenting therapeutic effects. This study that takes advantage of defect engineering offers new insights into developing high-efficiency redox nanozymes.
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