Ruthenium Single-Atom Nanozyme Driven Sonosensitizer with Oxygen Vacancies Enhances Electron-Hole Separation Efficacy and Remodels Tumor Microenvironment for Sonodynamic-Amplified Ferroptosis

被引:3
作者
Zhu, Yang [1 ,2 ]
Wang, Dengliang [1 ,2 ]
Du, Chengzhong [1 ,2 ]
Wu, Tiantian [3 ]
Wei, Penghui [1 ,2 ]
Zheng, Hongjia [1 ,2 ]
Li, Guanting [1 ,2 ]
Zheng, ShunZhe [1 ,2 ]
Su, Lichao [1 ,2 ]
Yan, Lingjun [1 ,2 ]
Hu, Yongrui [1 ,2 ]
Wang, Huimin [1 ,2 ]
Lin, Lisen [1 ,2 ]
Ding, Chenyu [1 ,2 ]
Chen, Xiaoyuan [4 ,5 ,6 ,7 ,8 ,9 ,10 ]
机构
[1] Fujian Med Univ, Affiliated Hosp 1, Neurosurg Res Inst, Dept Neurosurg, Fuzhou 350209, Fujian, Peoples R China
[2] Fujian Med Univ, Affiliated Hosp 1, Natl Reg Med Ctr, Dept Neurosurg, Binhai Campus, Fuzhou 350212, Fujian, Peoples R China
[3] Hainan Med Univ, Sch Pharmaceut Sci, Sch Trop Med, NHC Key Lab Trop Dis Control, Haikou 571199, Peoples R China
[4] Natl Univ Singapore, Yong Loo Lin Sch Med, Dept Diagnost Radiol, Singapore 119074, Singapore
[5] Natl Univ Singapore, Yong Loo Lin Sch Med, Dept Surg, Singapore 119074, Singapore
[6] Natl Univ Singapore, Yong Loo Lin Sch Med, Dept Chem & Biomol Engn, Singapore 119074, Singapore
[7] Natl Univ Singapore, Yong Loo Lin Sch Med, Dept Biomed Engn, Singapore 119074, Singapore
[8] Natl Univ Singapore, Coll Design & Engn, Singapore 119074, Singapore
[9] Natl Univ Singapore, Clin Imaging Res Ctr, Ctr Translat Med, Yong Loo Lin Sch Med, Singapore 117599, Singapore
[10] Natl Univ Singapore, Yong Loo Lin Sch Med, Nanomed Translat Res Program, Singapore 117597, Singapore
基金
中国国家自然科学基金; 英国医学研究理事会;
关键词
ferroptosis; oxygen vacancy; single-atom nanozyme; sonodynamic therapy; tumor microenvironment; THERAPY;
D O I
10.1002/advs.202416997
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Sonodynamic therapy (SDT) has emerged as a promising noninvasive approach for tumor therapy. However, the effectiveness of traditional inorganic semiconductor sonosensitizers is hindered by rapid electron (e-) and hole (h+) recombination under ultrasonic (US) stimulation, as well as the hypoxic and reductive conditions of tumor microenvironment (TME), which limit the generation of reactive oxygen species (ROS). Herein, a ruthenium (Ru) single-atom nanozyme-driven superimposition-enhanced titanium dioxide-based sonosensitizer (Ru/TiO2-x SAE) is presented that features sufficient oxygen vacancies and high e-/h+ separation efficiency. Through synchrotron radiation-based X-ray absorption spectroscopy and extended X-ray absorption fine structure analysis it is confirmed that oxygen vacancies in TiO2-x nanoparticles promote the immobilization of single-atomic Ru, forming Ru-O-4 active sites. Density functional theory calculations demonstrate that oxygen vacancies alter the electronic structure of nanosensitizer, enhanced e-/h+ separation, increasing oxygen adsorption, and accelerating reaction kinetics under US stimulation, ultimately improving ROS production. Moreover, Ru/TiO2-x SAE boosts sonodynamic efficacy by mitigating the hypoxic and reductive TME. This is attributed to its catalase- and glutathione peroxidase 4-like activities, which facilitate the generation of ROS and trigger lipid peroxidation-mediated ferroptosis. These findings highlight the innovative role of single-atom Ru in optimizing sonosensitizers for SDT-induced ferroptosis, demonstrating its potential for advancing cancer therapy.
引用
收藏
页数:13
相关论文
共 63 条
[1]   How to Build Plasmon-Driven Molecular Jackhammers that Disassemble Cell Membranes and Cytoskeletons in Cancer [J].
Ayala-Orozco, Ciceron ;
Li, Gang ;
Li, Bowen ;
Vardanyan, Vardan ;
Kolomeisky, Anatoly B. ;
Tour, James M. .
ADVANCED MATERIALS, 2024, 36 (14)
[2]   Ultrasmall Iron-Doped Titanium Oxide Nanodots for Enhanced Sonodynamic and Chemodynamic Cancer Therapy [J].
Bai, Shang ;
Yang, Nailin ;
Wang, Xianwen ;
Gong, Fei ;
Dong, Ziliang ;
Gong, Yuehan ;
Liu, Zhuang ;
Cheng, Liang .
ACS NANO, 2020, 14 (11) :15119-15130
[3]   Piezoelectric Metal-Organic Frameworks Based Sonosensitizer for Enhanced Nanozyme Catalytic and Sonodynamic Therapies [J].
Cai, Lihan ;
Du, Jianjun ;
Han, Fuping ;
Shi, Tiancong ;
Zhang, Han ;
Lu, Yang ;
Long, Saran ;
Sun, Wen ;
Fan, Jiangli ;
Peng, Xiaojun .
ACS NANO, 2023, 17 (08) :7901-7910
[4]   Defect-Engineering Bismuth-Based Homologous Schottky Heterojunction for Metabolic Regulation-Augmented Sonodynamic Tumor Therapy [J].
Cao, Xinyue ;
Wang, Ying ;
Song, Xinran ;
Lou, Wanqing ;
Li, Xiaoyan ;
Lu, Weiping ;
Chen, Kai ;
Chen, Liang ;
Chen, Yu ;
Huang, Bingcang .
ADVANCED FUNCTIONAL MATERIALS, 2023, 33 (25)
[5]   Engineering Heterostructured Piezoelectric Nanorods with Rich Oxygen Vacancy-Mediated Piezoelectricity for Ultrasound-Triggered Piezocatalytic Cancer Therapy [J].
Chen, Wenying ;
Chen, Qi ;
Song, Feifei ;
Hua, Mengying ;
Chang, Meiqi ;
Feng, Wei ;
Ding, Li ;
Yang, Bin ;
Chen, Yu ;
Hu, Zhongqian .
ADVANCED FUNCTIONAL MATERIALS, 2024, 34 (41)
[6]   Enhanced Photocatalytic and Photovoltaic Performance Arising from Unconventionally Low Donor-Y6 Ratios [J].
Dolan, Andrew ;
Pan, Xun ;
Griffith, Matthew J. ;
Sharma, Anirudh ;
de la Perrelle, Jessica M. ;
Baran, Derya ;
Metha, Gregory F. ;
Huang, David M. ;
Kee, Tak W. ;
Andersson, Mats R. .
ADVANCED MATERIALS, 2024, 36 (15)
[7]   2D Piezoelectric Bi2MoO6 Nanoribbons for GSH-Enhanced Sonodynamic Therapy [J].
Dong, Yushan ;
Dong, Shuming ;
Liu, Bin ;
Yu, Chenghao ;
Liu, Jing ;
Yang, Dan ;
Yang, Piaoping ;
Lin, Jun .
ADVANCED MATERIALS, 2021, 33 (51)
[8]  
Dong ZL, 2020, CHEM-US, V6, P1391, DOI 10.1016/j.chempr.2020.02.020
[9]   In vivo guiding nitrogen-doped carbon nanozyme for tumor catalytic therapy [J].
Fan, Kelong ;
Xi, Juqun ;
Fan, Lei ;
Wang, Peixia ;
Zhu, Chunhua ;
Tang, Yan ;
Xu, Xiangdong ;
Liang, Minmin ;
Jiang, Bing ;
Yan, Xiyun ;
Gao, Lizeng .
NATURE COMMUNICATIONS, 2018, 9
[10]   Single Atom Catalysts Remodel Tumor Microenvironment for Augmented Sonodynamic Immunotherapy [J].
Geng, Bijiang ;
Hu, Jinyan ;
He, Xialing ;
Zhang, Zhenlin ;
Cai, Jinming ;
Pan, Dengyu ;
Shen, Longxiang .
ADVANCED MATERIALS, 2024, 36 (25)