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Silicon doping-engineered asymmetric coordination and electronic structure modulation for amplified single-atom
Bo Liu1,2, Huihan Yi1,2, Zhan Zhuang1,2
1Fujian Key Laboratory of Precision Medicine for Cancer, Department of Thoracic Surgery, The First Affiliated Hospital, Fujian Medical University, Fuzhou, 350005, China.
Materials Today. Bio
|April 20, 2026
Summary
Engineered single-atom nanozymes with asymmetric coordination and silicon doping show enhanced catalytic activity. This breakthrough improves reactive oxygen species generation for inducing tumor ferroptosis.
Area of Science:
- Biomedical Engineering
- Materials Science
- Nanotechnology
Background:
- Single-atom nanozymes (SANs) offer tunable properties but lag behind natural enzymes in catalytic performance due to symmetric structures.
- Optimizing coordination environments is key to enhancing SAN catalytic efficiency for biomedical applications.
Purpose of the Study:
- To engineer an asymmetrically coordinated Fe-based SAN with Si doping (Fe-SiN3/SAN) for superior catalytic activity.
- To investigate the mechanism behind the enhanced performance of Fe-SiN3/SAN compared to symmetric Fe-N4/SAN.
- To evaluate the efficacy of Fe-SiN3/SAN in inducing tumor ferroptosis.
Main Methods:
- Fabrication of an asymmetrically coordinated Fe-based SAN with Si doping.
- Utilizing Density Functional Theory (DFT) calculations to analyze electronic structures and coordination effects.
- Conducting experimental validation of catalytic activity and tumor ferroptosis induction.
Main Results:
- Fe-SiN3/SAN demonstrated significantly enhanced catalytic performance over Fe-N4/SAN.
- DFT analysis revealed that asymmetric coordination optimizes oxygen intermediate adsorption/desorption and enhances electron activation.
- Fe-SiN3/SAN effectively induced irreversible tumor ferroptosis by promoting lipid peroxidation and inhibiting glutathione peroxidase 4.
Conclusions:
- Asymmetric coordination and Si doping in Fe-based SANs can substantially boost catalytic activity.
- Fe-SiN3/SAN shows promise as an effective agent for cancer therapy via ferroptosis induction.
