材料科学
电子转移
自旋极化
极化(电化学)
纳米技术
电荷(物理)
电子
化学工程
化学物理
光化学
物理化学
量子力学
物理
工程类
化学
作者
Juan Guo,Xueting Pan,Chaohui Wang,Zhijun Huang,Zezhong Huang,Jingqian Deng,Qingyuan Wu,Yun Sun,Xican Xu,Dandan Hou,Huiyu Liu
出处
期刊:PubMed
日期:2025-09-09
卷期号:: e06721-e06721
标识
DOI:10.1002/adma.202506721
摘要
Sonocatalytic therapy (SCT) is a non-invasive tumor treatment modality that utilizes ultrasound (US)- activated sonocatalysts to generate reactive oxygen species (ROS), whose production critically dependent on the electronic structural properties of the catalytic sites. However, the spin state, which is a pivotal descriptor of electronic properties, remains underappreciated in SCT. Herein, a Ti-doped zirconium-based MOF (Ti-UiO-66, denoted as UTN) with ligand-deficient defects is constructed for SCT, revealing the important role of the electronic spin state in modulating intrinsic catalytic activity. The defect-driven sonocatalytic mechanism is elucidated as follows: 1) structural defects alleviate the limitations of ligand-metal charge transfer, achieving a 2.1-fold enhancement in charge transfer efficiency; 2) spin polarization at Ti active sites reconfigures the d-orbital electron distribution, thereby increasing the density of spin-polarized electronic states near the Fermi level. Furthermore, Ti 3d-O 2p orbital hybridization lowers the adsorption energies of H2O and O2 by 2.5-fold and 1.6-fold, respectively, thereby facilitating interfacial redox reactions and leading to enhanced ROS generation. Notably, UTN combined with US achieves 86.07% tumor inhibition efficiency. This work establishes novel insights into defect engineering, spin-state modulation, and surface interfacial adsorption in SCT, providing a theoretical paradigm framework for designing of high-performance sonocatalysts.
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