Embedding Atomically Dispersed Manganese/Gadolinium Dual Sites in Oxygen Vacancy-Enriched Biodegradable Bimetallic Silicate Nanoplatform for Potentiating Catalytic Therapy.

Jin Ye, Kefen Zhang, Xing Yang, Mengting Liu, Yujie Cui, Yunlong Li, Chunsheng Li, Shuang Liu, Yong Lu, Zhiyong Zhang, Na Niu, Ligang Chen, Yujie Fu, Jiating Xu

Journal: Advanced science (Weinheim, Baden-Wurttemberg, Germany) 2024;11(4):e2307424

PMID: 38037255

Abstract

Due to their atomically dispersed active centers, single-atom nanozymes (SAzymes) have unparalleled advantages in cancer catalytic therapy. Here, loaded with chlorin e6 (Ce6), a hydrothermally mass-produced bimetallic silicate-based nanoplatforms with atomically dispersed manganese/gadolinium (Mn/Gd) dual sites and oxygen vacancies (OVs) (PMn GMSNs-V@Ce6) is constructed for tumor glutathione (GSH)-triggered chemodynamic therapy (CDT) and O -alleviated photodynamic therapy. The band gaps of silica are significantly reduced from 2.78 to 1.88 eV by doping with metal ions, which enables it to be excited by a 650 nm laser to produce electron-hole pairs, thereby facilitating the generation of reactive oxygen species. The Gd sites can modulate the local electrons of the atom-catalyzed Mn sites, which contribute to the generation of superoxide and hydroxyl radicals ( OH). Tumor GSH-triggered Mn release can convert endogenous H O to OH and realize GSH-depletion-enhanced CDT. Significantly, the hydrothermally generated OVs can not only capture Mn and Gd atoms to form atomic sites but also can elongate and weaken the O-O bonds of H O , thereby improving the efficacy of Fenton reactions. The degraded Mn /Gd ions can be used as tumor-specific magnetic resonance imaging contrast agents. All the experimental results demonstrate the great potential of PMn GMSNs-V@Ce6 as cancer theranostic agent.

© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.

Address: Key Laboratory of Forest Plant Ecology, Ministry of Education College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin, 150001, P. R. China.; The Second Affiliated Hospital, Heilongjiang Provincial Key Laboratory of Ecological Utilization of Forestry-Based Active Substances, Northeast Forestry University, Harbin, 150040, P. R. China.; Guangxi University of Science and Technology, Liuzhou, 545006, P. R. China.; School of Laboratory Medicine, Wannan Medical College, Wuhu, Anhui, 241002, P.R. China.; College of Biological Sciences and Technology, Beijing Forestry University, Beijing, 100083, P.R. China.
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