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Research Article

Asymmetrically coordinated single-atom iron nanozymes with Fe-N1C2 structure: A peroxidase mimetic for melatonin detection

Lihong Lin1,§, Heng Li2,§, Hongfei Gu1,§, Zhiyi Sun1, Juan Huang2, Zhenni Qian2, Hang Li1, Juzhe Liu3, Hongyan Xi4, Pengfei Wu4, Qingqing Liu4, Shuhu Liu5, Lirong Zheng5, Zhuo Chen1(), Zhengbo Chen2(), Juanjuan Qi3()
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemistry, Capital Normal University, Beijing 100081, China
The Key Laboratory of Resources and Environmental System Optimization, Ministry of Education (MOE), College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
School of Chemistry, Beihang University, Beijing 100191, China
Institute of High Energy Physics, Chinese Academy of Science, Beijing 100049, China

§ Lihong Lin, Heng Li, and Hongfei Gu contributed equally to this work.

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Graphical Abstract

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By introducing highly electronegative N atoms to optimize the local coordination environment of Fe atoms, it is expected to enhance the catalytic activity towards peroxide substrates. Compared with the single-atom Fe nanozyme anchored on undoped Ti3C2Tx (Fe SA/Ti3C2Tx), Fe SA/N-Ti3C2Tx with Fe-N1C2 structure exhibits higher catalytic activity and dynamics for 3,3’,5,5’-tetramethylbenzidine (TMB).

Abstract

Owing to the unique coordination environment and high atom utilization efficiency, single atom catalysts have been considered as an ideal artificial enzyme to mimic natural enzymes. Herein, single-atom Fe nanozyme anchored on N-doped Ti3C2Tx (Fe SA/N-Ti3C2Tx) with asymmetrically coordinated Fe-N1C2 configuration is synthesized by vacancy capture and heteroatom doping strategy, which exhibits excellent peroxidase-like activity. Based on the results of peroxidase catalytic kinetics and X-ray adsorption fine spectroscopy, the Fe-N1C2 active sites in Fe SA/N-Ti3C2Tx are responsible for the excellent performance. Furthermore, the developed Fe SA/N-Ti3C2Tx can be employed to quantitative detection of melatonin (MT), which shows a wide linear detection range (0.01–100 μM) and an excellent detection limit (7.3 nM) in buffer, 0.01–100 μM and 7.8 nM in serum samples. Our work proves that MXene-based single atoms can be promising nanozyme in the field of bioassays.

Keywords

iron single atomasymmetric coordinationTi3C2Tx MXenenanozymemelatonin detection

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Nano Research
Volume 16 Issue 4,
April 2023
Pages 4751-4757
DOI: 10.1007/s12274-022-5211-8
Cite this article:
Lin L, Li H, Gu H, et al. Asymmetrically coordinated single-atom iron nanozymes with Fe-N1C2 structure: A peroxidase mimetic for melatonin detection. Nano Research, 2023, 16(4): 4751-4757. https://doi.org/10.1007/s12274-022-5211-8
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