Axial O Atom-Modulated Fe(III)-N4 Sites for Enhanced Cascade Catalytic 1O2-Induced Tumor Therapy
文献类型:期刊论文
作者 | Liu, Hongji1,7; Yu, Biao2,3,7![]() ![]() |
刊名 | ADVANCED SCIENCE
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出版日期 | 2024-07-01 |
关键词 | axial O coordination cascade catalytic therapy ferroptosis iron single atom nanozymes singlet oxygen |
DOI | 10.1002/advs.202307254 |
通讯作者 | Zhang, Xin(xinzhang@hmfl.ac.cn) ; Wang, Kai(hyxj0309@163.com) ; Wang, Hui(hw39@hmfl.ac.cn) |
英文摘要 | The rational construction of efficient hypoxia-tolerant nanocatalysts capable of generating singlet oxygen (O-1(2)) without external stimuli is of great importance for tumor therapy. Herein, uniformly dispersed and favorable biosafety profile graphitic carbon nitride quantum dots immobilized with Fe-N-4 moieties modulated by axial O atom (denoted as O-Fe-N-4) are developed for converting H2O2 into O-1(2) via Russell reaction, without introducing external energy. Notably, O-Fe-N-4 performs two interconnected catalytic properties: glutathione oxidase-mimic activity to provide substrate for subsequent O-1(2) generation, avoiding the blunting anticancer efficacy by glutathione. The O-Fe-N-4 catalyst demonstrates a specific activity of 79.58 U mg(-1) at pH 6.2, outperforming the most reported Fe-N-4 catalysts. Density functional theory calculations demonstrate that the axial O atom can effectively modulate the relative position and electron affinity between Fe and N, lowering the activation energy, strengthening the selectivity, and thus facilitating the Russell-type reaction. The gratifying enzymatic activity stemming from the well-defined Fe-N/O structure can inhibit tumor proliferation by efficiently downregulating glutathione peroxidase 4 activity and inducing lipid peroxidation. Altogether, the O-Fe-N-4 catalyst not only represents an efficient platform for self-cascaded catalysis to address the limitations of O-1(2)-involved cancer treatment but also provides a paradigm to enhance the performance of the Fe-N-4 catalyst. |
资助项目 | National Key R&D Program of China[2021YFA1600202] ; China National Postdoctoral Program for Innovative Talents[BX20230111] ; National Natural Science Foundation of China[U21A20148] ; Anhui Provincial Natural Science Foundation[2308085J18] ; CASHIPS Director's Fund[YZJJ2023QN43] ; China Post-doctoral Science Foundation[2023M743536] ; High Magnetic Field Laboratory of Anhui Province ; Science Research Fund for Post-doctoral in Anhui Province[2023B669] |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science |
语种 | 英语 |
WOS记录号 | WOS:001259676300001 |
出版者 | WILEY |
资助机构 | National Key R&D Program of China ; China National Postdoctoral Program for Innovative Talents ; National Natural Science Foundation of China ; Anhui Provincial Natural Science Foundation ; CASHIPS Director's Fund ; China Post-doctoral Science Foundation ; High Magnetic Field Laboratory of Anhui Province ; Science Research Fund for Post-doctoral in Anhui Province |
源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/136747] ![]() |
专题 | 中国科学院合肥物质科学研究院 |
通讯作者 | Zhang, Xin; Wang, Kai; Wang, Hui |
作者单位 | 1.Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China 2.Anhui Med Univ, Affiliated Hosp 1, Dept Obstet & Gynecol, Hefei 230022, Anhui, Peoples R China 3.Anhui Med Univ, NHC Key Lab Study Abnormal Gametes & Reprod Tract, Hefei 230022, Anhui, Peoples R China 4.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei 230026, Peoples R China 5.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China 6.Nanjing Univ, Sch Life Sci, State Key Lab Pharmaceut Biotechnol, Nanjing 210023, Jiangsu, Peoples R China 7.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Anhui, Peoples R China |
推荐引用方式 GB/T 7714 | Liu, Hongji,Yu, Biao,Yang, Pengqi,et al. Axial O Atom-Modulated Fe(III)-N4 Sites for Enhanced Cascade Catalytic 1O2-Induced Tumor Therapy[J]. ADVANCED SCIENCE,2024. |
APA | Liu, Hongji.,Yu, Biao.,Yang, Pengqi.,Yang, Yang.,Deng, Zhiming.,...&Wang, Hui.(2024).Axial O Atom-Modulated Fe(III)-N4 Sites for Enhanced Cascade Catalytic 1O2-Induced Tumor Therapy.ADVANCED SCIENCE. |
MLA | Liu, Hongji,et al."Axial O Atom-Modulated Fe(III)-N4 Sites for Enhanced Cascade Catalytic 1O2-Induced Tumor Therapy".ADVANCED SCIENCE (2024). |
入库方式: OAI收割
来源:合肥物质科学研究院
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