Bioinspired porous three-coordinated single-atom Fe nanozyme with oxidase-like activity for tumor visual identification via glutathione

被引:99
作者
Chen, Da [1 ]
Xia, Zhaoming [2 ]
Guo, Zhixiong [1 ]
Gou, Wangyan [1 ]
Zhao, Junlong [3 ]
Zhou, Xuemei [4 ]
Tan, Xiaohe [1 ]
Li, Wenbin [1 ]
Zhao, Shoujie [3 ]
Tian, Zhimin [1 ]
Qu, Yongquan [1 ]
机构
[1] Northwestern Polytech Univ, Sch Chem & Chem Engn, Key Lab Special Funct & Smart Polymer Mat, Minist Ind & Informat Technol, Xian 710072, Peoples R China
[2] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
[3] Fourth Mil Med Univ, Dept Med Genet & Dev Biol, State Key Lab Canc Biol, Xian 710032, Peoples R China
[4] Wenzhou Univ, Key Lab Carbon Mat Zhejiang Prov, Wenzhou 325035, Peoples R China
基金
中国国家自然科学基金;
关键词
OXYGEN REDUCTION; IRON; ELECTROCATALYST; SITES;
D O I
10.1038/s41467-023-42889-w
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Inspired by structures of natural metalloenzymes, a biomimetic synthetic strategy is developed for scalable synthesis of porous Fe-N-3 single atom nanozymes (pFeSAN) using hemoglobin as Fe-source and template. pFeSAN delivers 3.3- and 8791-fold higher oxidase-like activity than Fe-N-4 and Fe3O4 nanozymes. The high catalytic performance is attributed to (1) the suppressed aggregation of atomically dispersed Fe; (2) facilitated mass transfer and maximized exposure of active sites for the created mesopores by thermal removal of hemoglobin (2 similar to 3 nm); and (3) unique electronic configuration of Fe-N-3 for the oxygen-to-water oxidation pathway (analogy with natural cytochrome c oxidase). The pFeSAN is successfully demonstrated for the rapid colorimetric detection of glutathione with a low limit of detection (2.4 nM) and wide range (50 nM-1 mM), and further developed as a real-time, facile, rapid (similar to 6 min) and precise visualization analysis methodology of tumors via glutathione level, showing its potentials for diagnostic and clinic applications.
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页数:13
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共 64 条
[1]   Designing Hierarchically Porous Single Atoms of Fe-N5 Catalytic Sites with High Oxidase-like Activity for Sensitive Detection of Organophosphorus Pesticides [J].
Chen, Tiantian ;
Zhou, Dandan ;
Hou, Shenghuai ;
Li, Yan ;
Liu, Ying ;
Zhang, Manlin ;
Zhang, Ganbing ;
Xu, Hui .
ANALYTICAL CHEMISTRY, 2022, :15270-15279
[2]   Quantitative evaluation of O2 activation half-reaction for Fe-N-C in oxidase-like activity enhancement [J].
Chen, Xinghua ;
Zhu, Caixia ;
Xu, Yuan ;
Wang, Kaiyuan ;
Cao, Xuwen ;
Shen, Yanfei ;
Liu, Songqin ;
Zhang, Yuanjian .
CATALYSIS SCIENCE & TECHNOLOGY, 2021, 11 (22) :7255-7259
[3]   Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction [J].
Chen, Yuanjun ;
Ji, Shufang ;
Wang, Yanggang ;
Dong, Juncai ;
Chen, Wenxing ;
Li, Zhi ;
Shen, Rongan ;
Zheng, Lirong ;
Zhuang, Zhongbin ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (24) :6937-6941
[4]   GSH-Depleted Nanozymes with Hyperthermia-Enhanced Dual Enzyme-Mimic Activities for Tumor Nanocatalytic Therapy [J].
Dong, Shuming ;
Dong, Yushan ;
Jia, Tao ;
Liu, Shikai ;
Liu, Jing ;
Yang, Dan ;
He, Fei ;
Gai, Shili ;
Yang, Piaoping ;
Lin, Jun .
ADVANCED MATERIALS, 2020, 32 (42)
[5]   Surface Ligand Engineering Ruthenium Nanozyme Superior to Horseradish Peroxidase for Enhanced Immunoassay [J].
Fan, Huizhen ;
Zheng, Jiajia ;
Xie, Jiaying ;
Liu, Juewen ;
Gao, Xingfa ;
Yan, Xiyun ;
Fan, Kelong ;
Gao, Lizeng .
ADVANCED MATERIALS, 2024, 36 (10)
[6]   Nanocatalytic Theranostics with Glutathione Depletion and Enhanced Reactive Oxygen Species Generation for Efficient Cancer Therapy [J].
Fu, Lian-Hua ;
Wan, Yilin ;
Qi, Chao ;
He, Jin ;
Li, Chunying ;
Yang, Chen ;
Xu, Han ;
Lin, Jing ;
Huang, Peng .
ADVANCED MATERIALS, 2021, 33 (07)
[7]   Computational Design of Spinel Oxides through Coverage-Dependent Screening on the Reaction Phase Diagram [J].
Guo, Chenxi ;
Tian, Xin ;
Fu, Xiaoyan ;
Qin, Gangqiang ;
Long, Jun ;
Li, Huan ;
Jing, Huijuan ;
Zhou, Yonghua ;
Xiao, Jianping .
ACS CATALYSIS, 2022, 12 (11) :6781-6793
[8]   Theoretical Insights on the Synergy and Competition between Thermochemical and Electrochemical Steps in Oxygen Electroreduction [J].
Guo, Chenxi ;
Fu, Xiaoyan ;
Xiao, Jianping .
JOURNAL OF PHYSICAL CHEMISTRY C, 2020, 124 (47) :25796-25804
[9]   A two-dimensional thin Co-MOF nanosheet as a nanozyme with high oxidase-like activity for GSH detection [J].
Han, Miaomiao ;
Ren, Mengzhen ;
Li, Zhaohui ;
Qu, Lingbo ;
Yu, Lanlan .
NEW JOURNAL OF CHEMISTRY, 2022, 46 (22) :10682-10689
[10]   Ultrasensitive Detection of Bacteria Using a 2D MOF Nanozyme-Amplified Electrochemical Detector [J].
Hu, Wen-Chao ;
Pang, Jie ;
Biswas, Sudip ;
Wang, Kang ;
Wang, Chen ;
Xia, Xing-Hua .
ANALYTICAL CHEMISTRY, 2021, 93 (24) :8544-8552