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Nano Research 2023, 16(7): 10053-10060 https://doi.org/10.1007/s12274-023-5739-2
Research Article | Issue | Published: 13 May 2023

Peroxidase-like single Fe atoms anchored on Ti3C2Tx MXene as surface enhanced Raman scattering substrate for the simultaneous discrimination of multiple antioxidants

Show Author's Information Hongyan Xi1,§,  Hongfei Gu2,§,  Yurui Han3,§,  Tingting You1,  Pengfei Wu1,  Qingqing Liu1,  Lirong Zheng4,  Shuhu Liu4,  Qiang Fu5,  Wenxing Chen2,  Yukun Gao1,  Yuting Wang1( ),  Penggang Yin1( )
Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemical Physics, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China
Institute of High Energy Physics, Chinese Academy of Science, Beijing 100029, China
School of Future Technology, University of Science and Technology of China, Hefei 230026, China

§ Hongyan Xi, Hongfei Gu, and Yurui Han contributed equally to this work.

Keywords:
single atom catalyst, surface enhanced Raman scattering (SERS), Ti3C2Tx MXene, antioxidants, atomic interface site
Topics:
Raman spectroscopy
Cite this article:
Xi H, Gu H, Han Y, et al. Peroxidase-like single Fe atoms anchored on Ti3C2Tx MXene as surface enhanced Raman scattering substrate for the simultaneous discrimination of multiple antioxidants. Nano Research, 2023, 16(7): 10053-10060. https://doi.org/10.1007/s12274-023-5739-2
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Abstract Full text Electronic supplementary material About this article

Single-atom nanozymes (SAzymes) are emerging as promising alternatives to mimic natural enzyme, which is due to high atomic utilization efficiency, well-defined geometric, and unique electronic structure. Herein, Fe single atoms supported on Ti3C2Tx (Fe-SA/Ti3C2Tx) with intrinsic peroxidase activity is developed, further constructing a sensitive Raman sensor array for sensing of five antioxidants. Fe-SA/Ti3C2Tx shows excellent peroxidase-like performance in catalyzing the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) with colorimetric reactions. X-ray adsorption fine structure (XAFS) reveals that the electron transport between the Ti3C2Tx and Fe atoms occurs along Fe-O-Ti ligands, meanwhile the density functional theory (DFT) calculations confirm the spontaneous dissociation of H2O2 and the formation of OH radicals. Furthermore, the peroxidase-like Fe-SA/Ti3C2Tx was used as surface enhanced Raman scattering (SERS) substrate of oxidized TMB (TMB+) and achieved satisfied signal amplification performance. Using the blocking effects of free radical reactions, one-off identification of 5 antioxidants, including ascorbic acid (AA), uric acid (UA), glutathione (GSH), melatonin (Mel), and tea polyphenols (TPP), could be realized with this high identifiable catalytic property. This principle could realize 100% distinguish accuracy combined with linear discriminant analysis (LDA) and heat map data analysis. A wide detection concentration ranges from 10−8 to 10−3 M for five antioxidants was also achieved.


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Electronic supplementary material
About this article

Peroxidase-like single Fe atoms anchored on Ti3C2Tx MXene as surface enhanced Raman scattering substrate for the simultaneous discrimination of multiple antioxidants

Show Author's information Hongyan Xi1,§, Hongfei Gu2,§, Yurui Han3,§, Tingting You1, Pengfei Wu1, Qingqing Liu1, Lirong Zheng4, Shuhu Liu4, Qiang Fu5, Wenxing Chen2, Yukun Gao1, Yuting Wang1( ), Penggang Yin1( )
Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing 100191, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemical Physics, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China
Institute of High Energy Physics, Chinese Academy of Science, Beijing 100029, China
School of Future Technology, University of Science and Technology of China, Hefei 230026, China

§ Hongyan Xi, Hongfei Gu, and Yurui Han contributed equally to this work.

Abstract

Single-atom nanozymes (SAzymes) are emerging as promising alternatives to mimic natural enzyme, which is due to high atomic utilization efficiency, well-defined geometric, and unique electronic structure. Herein, Fe single atoms supported on Ti3C2Tx (Fe-SA/Ti3C2Tx) with intrinsic peroxidase activity is developed, further constructing a sensitive Raman sensor array for sensing of five antioxidants. Fe-SA/Ti3C2Tx shows excellent peroxidase-like performance in catalyzing the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) with colorimetric reactions. X-ray adsorption fine structure (XAFS) reveals that the electron transport between the Ti3C2Tx and Fe atoms occurs along Fe-O-Ti ligands, meanwhile the density functional theory (DFT) calculations confirm the spontaneous dissociation of H2O2 and the formation of OH radicals. Furthermore, the peroxidase-like Fe-SA/Ti3C2Tx was used as surface enhanced Raman scattering (SERS) substrate of oxidized TMB (TMB+) and achieved satisfied signal amplification performance. Using the blocking effects of free radical reactions, one-off identification of 5 antioxidants, including ascorbic acid (AA), uric acid (UA), glutathione (GSH), melatonin (Mel), and tea polyphenols (TPP), could be realized with this high identifiable catalytic property. This principle could realize 100% distinguish accuracy combined with linear discriminant analysis (LDA) and heat map data analysis. A wide detection concentration ranges from 10−8 to 10−3 M for five antioxidants was also achieved.

Keywords: single atom catalyst, surface enhanced Raman scattering (SERS), Ti3C2Tx MXene, antioxidants, atomic interface site

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Publication history
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Acknowledgements

Publication history

Received: 04 March 2023
Revised: 10 April 2023
Accepted: 13 April 2023
Published: 13 May 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51872011, 51902011, and 22005013), Beijing Natural Science Foundation (No. 2212018), Beijing Institute of Technology Research Fund Program for Young Scholars (No. 2022CX01011), and Chinese Academy of Sciences. The authors thank the BL1W1B and 4B7B in the Beijing Synchrotron Radiation Facility (BSRF) for help with characterizations.

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