Coordinately unsaturated single Fe-atoms with N vacancies and enhanced sp3 carbon defects in Fe-N(sp2)-C structural units for suppression of cancer cell metabolism and electrochemical oxygen evolution

被引:0
|
作者
Yadav, Anubha [1 ]
Hiremath, Netra [2 ]
Saini, Bhagirath [4 ]
Matsagar, Babasaheb M. [5 ]
Han, Po-Chun [5 ]
Ujihara, Masaki [6 ]
Modi, Mohammed Hussein [7 ]
Wu, Kevin C. -W. [5 ,8 ]
Sharma, Rakesh K. [4 ]
Vankayala, Raviraj [2 ,3 ]
Dutta, Saikat [1 ]
机构
[1] Amity Univ, Amity Inst Click Chem Res & Studies, Electrochem Energy & Sensor Res Lab, Noida, India
[2] Indian Inst Technol Jodhpur, Interdisciplinary Res Platform Smart Healthcare, Karwar 342030, Rajasthan, India
[3] Indian Inst Technol Jodhpur, Dept Biosci & Bioengn, Nanomed Lab, Karwar 342030, Rajasthan, India
[4] Indian Inst Technol Jodhpur, Dept Chem, Sustainable Mat & Catalysis Res Lab SMCRL, Jodhpur, India
[5] Natl Taiwan Univ, Dept Chem Engn, Taipei 10617, Taiwan
[6] Natl Taiwan Univ Sci & Technol, Grad Inst Appl Sci & Technol, Taipei, Taiwan
[7] Raja Ramanna Ctr Adv Technol, Synchrotron Utilizat Sect, Soft Xray Applicat Lab, Indore, India
[8] Yuan Ze Univ, Dept Chem Engn & Mat Sci, Taoyuan, Taiwan
关键词
ELECTROCATALYSTS; NANOTUBES;
D O I
10.1039/d4nr02553a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Installing coordinately unsaturated Fe-N-C structural units on polymer-composite-derived N-doped carbon offers highly active Fe-Nx sites for the electrochemical oxygen evolution reaction (OER) and reactive oxygen species (ROS) generation in tumor cells. An NH4Cl-driven high-temperature etching method was employed for the formation of FeSA950NC with coordinately unsaturated single Fe-atoms in an Fe-N(sp2)-C structural unit together with N vacancies (V-N) and sp(3) defects. The carbonization of Fe-phen@ZIF-8 at 800 degrees C for 30 min under argon, followed by grinding Fe-ZIF-8@RF-urea with NH4Cl at 950 degrees C for 2 hours, resulted in sp(3) carbon defects and V-N sites with coordination unsaturation in Fe-Nx due to NH4Cl decomposition to NH3 and HCl, which produced substantial internal stress for etching the carbon matrix. FeSA950NC was used to treat both A549 lung cancer cells and NIH3T3 mouse fibroblast cells to determine its potential as an efficient tumor therapeutic strategy using the 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) and ROS assays. Additionally, FeSA950NC provided high stability and excellent OER activity through the Fe-N(sp2)-C structural unit on pyridinic nitrogen by delivering at a minimum overpotential of 300 mV, which is much lower than that of structurally similar Fe-atom sites. The significantly stronger ROS and OER activities of FeSA950NC suggested the role of V-N and sp(3)-carbon defects with coordinately unsaturated Fe-N2 sites in improving its catalytic performance.
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页码:21416 / 21430
页数:15
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