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Single atom catalysts have been recognized as potential catalysts to fabricate electrochemical biosensors, due to their unexpected catalytic selectivity and activity. Here, we designed and fabricated an ultrasensitive dopamine (DA) sensor based on the flower-like MoS2 embellished with single Ni site catalyst (Ni-MoS2). The limit of detection could achieve 1 pM in phosphate buffer solution (PBS, pH = 7.4), 1 pM in bovine serum (pH = 7.4), and 100 pM in artificial urine (pH = 6.8). The excellent sensing performance was attributed to the Ni single atom axial anchoring on the Mo atom in the MoS2 basal plane with the Ni-S3 structure. Both the experiment and density functional theory (DFT) results certify that this structural feature is more favorable for the adsorption and electron transfer of DA on Ni atoms. The high proportion of Ni active sites on MoS2 basal plane effectively enhanced the intrinsic electronic conductivity and electrochemical activity toward DA. The successful establishment of this sensor gives a new guide to expand the field of single atom catalyst in the application of biosensors.

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Publication history
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Acknowledgements

Publication history

Received: 27 June 2022
Revised: 20 July 2022
Accepted: 22 July 2022
Published: 15 August 2022
Issue date: January 2023

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by China Ministry of Science and Technology (No. 2021YFA1500404), the Anhui Provincial Natural Science Foundation (Nos. 2108085QB70 and 2108085UD06), the DNL Cooperation Fund, CAS (No. DNL201918), the Collaborative Innovation Program of Hefei Science Center, CAS(No. 2021HSC-CIP002), the Natural Science Foundation of Hefei, China (No. 2021044), the Fundamental Research Funds for the Central Universities (Nos. WK2060000004, WK2060000021, WK2060000025, KY2060000180, and KY2060000195), and the Fundamental Research Funds for the Central Universities (No. WK5290000003). This work was partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication. Thank the funding support from CAS Fujian Institute of Innovation. We acknowledge the Experimental Center of Engineering and Material Science in the University of Science and Technology of China. We thank the photoemission endstations BL1W1B in Beijing Synchrotron Radiation Facility (BSRF), BL14W1 in Shanghai Synchrotron Radiation Facility (SSRF), and BL10B and BL11U in National Synchrotron Radiation Laboratory (NSRL) for the help in characterizations. The DFT calculations in this work were performed at the Supercomputing Center of the University of Science and Technology of China. Special thanks go to the Instrumental Analysis Center of Shenzhen University (Lihu Campus).

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