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Herein, a novel interference-free surface-enhanced Raman spectroscopy (SERS) strategy based on magnetic nanoparticles (MNPs) and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine. A core-satellite SERS aptasensor was constructed by combining aptamer-decorated Fe3O4@Au MNPs (as the recognize probe for histamine) and complementary DNA-modified silver nanoparticles carrying 4-mercaptobenzonitrile (4-MBN) (Ag@4-MBN@Ag-c-DNA) as the SERS signal probe for the indirect detection of histamine. Under an applied magnetic field in the absence of histamine, the assembly gave an intense Raman signal at “Raman biological-silent” region due to 4-MBN. In the presence of histamine, the Ag@4-MBN@Ag-c-DNA SERS-tag was released from the Fe3O4@Au MNPs, thus decreasing the SERS signal. Under optimal conditions, an ultra-low limit of detection of 0.65 × 10-3 ng/mL and a linear range 10-2–105 ng/mL on the SERS aptasensor were obtained. The histamine content in four food samples were analyzed using the SERS aptasensor, with the results consistent with those determined by high performance liquid chromatography. The present work highlights the merits of indirect strategies for the ultrasensitive and highly selective SERS detection of small biological molecules in complex matrices.


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A core-satellite self-assembled SERS aptasensor containing a “biological-silent region” Raman tag for the accurate and ultrasensitive detection of histamine

Show Author's information Chen Chena,1Yingfang Zhanga,1Ximo Wanga,Xuguang QiaoaGeoffrey I.N. Waterhouseb( )Zhixiang Xua( )
Key Laboratory of Food Processing Technology and Quality Control in Shandong Province, College of Food Science and Engineering, Shandong Agricultural University, Tai’an 271018, China
School of Chemical Sciences, The University of Auckland, Auckland 1142, New Zealand

1 Yingfang Zhang and Chen Chen contributed equally to this work.

Peer review under responsibility of Tsinghua University Press.

Research Highlights

● A SERS aptasensor operating in “biological-silent region” was developed for histamine detection.

● This SERS strategy was based on magnetic-induced and aptamer-driven assemblies.

● Ag@4-MBN@Ag NPs were used to significantly amplify 4-mercaptobenzonitrile SERS signal.

● The linear range of aptasensor was 10-2–105 ng/mL, with a LOD of 0.65 × 10-3 ng/mL.

● The developed aptasensor allowed histamine quantification in a variety of foods.

Abstract

Herein, a novel interference-free surface-enhanced Raman spectroscopy (SERS) strategy based on magnetic nanoparticles (MNPs) and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine. A core-satellite SERS aptasensor was constructed by combining aptamer-decorated Fe3O4@Au MNPs (as the recognize probe for histamine) and complementary DNA-modified silver nanoparticles carrying 4-mercaptobenzonitrile (4-MBN) (Ag@4-MBN@Ag-c-DNA) as the SERS signal probe for the indirect detection of histamine. Under an applied magnetic field in the absence of histamine, the assembly gave an intense Raman signal at “Raman biological-silent” region due to 4-MBN. In the presence of histamine, the Ag@4-MBN@Ag-c-DNA SERS-tag was released from the Fe3O4@Au MNPs, thus decreasing the SERS signal. Under optimal conditions, an ultra-low limit of detection of 0.65 × 10-3 ng/mL and a linear range 10-2–105 ng/mL on the SERS aptasensor were obtained. The histamine content in four food samples were analyzed using the SERS aptasensor, with the results consistent with those determined by high performance liquid chromatography. The present work highlights the merits of indirect strategies for the ultrasensitive and highly selective SERS detection of small biological molecules in complex matrices.

Keywords: Aptamer, Surface-enhanced Raman spectroscopy, Raman biological-silent region, Histamine detection, Universal SERS-tag

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Publication history

Received: 29 August 2022
Revised: 08 October 2022
Accepted: 08 November 2022
Published: 25 September 2023
Issue date: March 2024

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© 2024 Beijing Academy of Food Sciences. Publishing services by Tsinghua University Press.

Acknowledgements

Acknowledgement

This work was financially supported by the National Natural Science Foundation of China (31972149). GINW acknowledges funding support from the MacDiarmid Institute for Advanced Materials and Nanotechnology and the Dodd-Walls Centre for Photonic and Quantum Technologies.

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This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

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