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Nano Research 2022, 15(3): 2722-2733 https://doi.org/10.1007/s12274-021-3741-0
Research Article | Issue | Published: 12 August 2021

Super-assembled sandwich-like Au@MSN@Ag nanomatrices for high-throughput and efficient detection of small biomolecules

Show Author's Information Dantong Zhao1,3,§,  Chunxia Ma2,§( ),  Meng Gao2,  Yong Li2,  Bo Yang2,  Hui Li1,  Runhao Zhang2,  Minglu Hao2,  Jing Huang2,  Kang Liang4,  Pu Chen5,  Lei Xie6,  Rong Rong1( ),  Biao Kong6( )
College of Medicine, Shandong University of Traditional Chinese Medicine, Jinan 250355, China
Shandong Analysis and Test Center, National Supercomputer Research Center of Advanced Materials, Advanced Materials Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250014, China
Heze Institute for Food and Drug Control, Heze 274000, China
School of Chemical Engineering and Graduate School of Biomedical Engineering, The University of New South Wales, NSW 2052, Australia
Department of Chemical Engineering, University of Waterloo, Waterloo, Ontario, N2L 3G1, Canada
Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200032, China

§Dantong Zhao and Chunxia Ma contributed equally to this work.

Keywords:
matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS), matrix, sandwich-like nanostructures, small biomolecules, traditional Chinese medicine (TCM)
Topics:
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Cite this article:
Zhao D, Ma C, Gao M, et al. Super-assembled sandwich-like Au@MSN@Ag nanomatrices for high-throughput and efficient detection of small biomolecules. Nano Research, 2022, 15(3): 2722-2733. https://doi.org/10.1007/s12274-021-3741-0
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Abstract Full text About this article

Small biomolecules (m/z < 500) are the material basis of organisms and participate in life activities, but their comprehensive and accurate detection in complex samples remains a challenge. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) is a powerful detection tool for molecular analysis with high throughput. The development of a new matrix is essential to improve the efficiency of the MALDI-MS for molecular compound detection. In this work, the sandwich-like gold nanoparticles@mesoporous silica nanocomposite@silver nanoparticles (Au@MSN@Ag) nanospheres were prepared by layer-by-layer super-assembly strategy, and can be used as a novel matrix for the quantitative detection and enrichment of small biomolecules by LDI-MS. The sandwich-like nanospheres form a unique plasma resonant cavity that effectively absorbs the laser energy, while the homogeneous mesoporous structure of MSN can lock the analyte, which is essential for efficient LDI of small molecules. Compared to traditional matrices, Au@MSN@Ag shows the advantages of low background, wide application range, high sensitivity, super high salt and protein tolerance, and good stability. For example, the detection limit of glucose was as low as 5 fmol, and showed a good linear relationship in the range of 1−750 μg/mL. Au@MSN@Ag assisted LDI-MS allows the enrichment and detection of small molecules in traditional Chinese medicine (TCM) without derivatization and purification, classification of herbs using the accurate quantitative results oligosaccharides, and identification of gelatin by amino acid content. This research could help in designing more efficient nanostructure matrices and further explored the application of LDI-MS.


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About this article

Super-assembled sandwich-like Au@MSN@Ag nanomatrices for high-throughput and efficient detection of small biomolecules

Show Author's information Dantong Zhao1,3,§, Chunxia Ma2,§( ), Meng Gao2, Yong Li2, Bo Yang2, Hui Li1, Runhao Zhang2, Minglu Hao2, Jing Huang2, Kang Liang4, Pu Chen5, Lei Xie6, Rong Rong1( ), Biao Kong6( )
College of Medicine, Shandong University of Traditional Chinese Medicine, Jinan 250355, China
Shandong Analysis and Test Center, National Supercomputer Research Center of Advanced Materials, Advanced Materials Institute, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250014, China
Heze Institute for Food and Drug Control, Heze 274000, China
School of Chemical Engineering and Graduate School of Biomedical Engineering, The University of New South Wales, NSW 2052, Australia
Department of Chemical Engineering, University of Waterloo, Waterloo, Ontario, N2L 3G1, Canada
Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, iChEM, Fudan University, Shanghai 200032, China

§Dantong Zhao and Chunxia Ma contributed equally to this work.

Abstract

Small biomolecules (m/z < 500) are the material basis of organisms and participate in life activities, but their comprehensive and accurate detection in complex samples remains a challenge. Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) is a powerful detection tool for molecular analysis with high throughput. The development of a new matrix is essential to improve the efficiency of the MALDI-MS for molecular compound detection. In this work, the sandwich-like gold nanoparticles@mesoporous silica nanocomposite@silver nanoparticles (Au@MSN@Ag) nanospheres were prepared by layer-by-layer super-assembly strategy, and can be used as a novel matrix for the quantitative detection and enrichment of small biomolecules by LDI-MS. The sandwich-like nanospheres form a unique plasma resonant cavity that effectively absorbs the laser energy, while the homogeneous mesoporous structure of MSN can lock the analyte, which is essential for efficient LDI of small molecules. Compared to traditional matrices, Au@MSN@Ag shows the advantages of low background, wide application range, high sensitivity, super high salt and protein tolerance, and good stability. For example, the detection limit of glucose was as low as 5 fmol, and showed a good linear relationship in the range of 1−750 μg/mL. Au@MSN@Ag assisted LDI-MS allows the enrichment and detection of small molecules in traditional Chinese medicine (TCM) without derivatization and purification, classification of herbs using the accurate quantitative results oligosaccharides, and identification of gelatin by amino acid content. This research could help in designing more efficient nanostructure matrices and further explored the application of LDI-MS.

Keywords: matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS), matrix, sandwich-like nanostructures, small biomolecules, traditional Chinese medicine (TCM)

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Publication history
Copyright
Acknowledgements

Publication history

Received: 03 May 2021
Revised: 29 June 2021
Accepted: 12 July 2021
Published: 12 August 2021
Issue date: March 2022

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (Nos. 2019YFC1604600, 2017YFA0206901, 2019YFC1604601, 2017YFA0206900, and 2018YFC1602301), the National Natural Science Foundation of China (Nos. 21705027, 21974029 51808328, 61903235, 42007218, and 51703109), the Major Scientific and Technological Innovation Project of Shandong (Nos. 2018CXGC1406, 2019JZZY010457 and 2019JZZY020309). The Natural Science Foundation of Shanghai (18ZR1404700), and Construction Project of Shanghai Key Laboratory of Molecular Imaging (18DZ2260400), Shanghai Municipal Education Commission (Class II Plateau Disciplinary Construction Program of Medical Technology of SUMHS, 2018-2020). The ability establishment of sustainable use for valuable Chinese medicine resources (2060302). The natural Science Foundation of Shandong Province, China (ZR2020QE228).

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