Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning

A major problem limiting reproducible use of liquid extraction surface analysis (LESA) array sampling of dried surface-deposited liquid samples is the unwanted spread of extraction solvent beyond the dried sample limits, resulting in unreliable data. Here, we explore the use of the Droplet Microarra...

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Main Authors: Meurs, Joris, Alexander, Morgan R., Levkin, Pavel A., Widmaier, Simon, Bunch, Josephine, Barrett, David A., Kim, Dong-Hyun
Format: Article
Published: American Chemical Society 2018
Online Access:https://eprints.nottingham.ac.uk/51621/
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author Meurs, Joris
Alexander, Morgan R.
Levkin, Pavel A.
Widmaier, Simon
Bunch, Josephine
Barrett, David A.
Kim, Dong-Hyun
author_facet Meurs, Joris
Alexander, Morgan R.
Levkin, Pavel A.
Widmaier, Simon
Bunch, Josephine
Barrett, David A.
Kim, Dong-Hyun
author_sort Meurs, Joris
building Nottingham Research Data Repository
collection Online Access
description A major problem limiting reproducible use of liquid extraction surface analysis (LESA) array sampling of dried surface-deposited liquid samples is the unwanted spread of extraction solvent beyond the dried sample limits, resulting in unreliable data. Here, we explore the use of the Droplet Microarray (DMA), which consists of an array of superhydrophilic spots bordered by a superhydrophobic material giving the potential to confine both the sample spot and the LESA extraction solvent in a defined area. We investigated the DMA method in comparison with a standard glass substrate using LESA analysis of a mixture of biologically relevant compounds with a wide mass range and different physicochemical properties. The optimized DMA method was subsequently applied to urine samples from a human intervention study. Relative standard deviations for the signal intensities were all reduced at least 3-fold when performing LESA-MS on the DMA surface compared with a standard glass surface. Principal component analysis revealed more tight clusters indicating improved spectral reproducibility for a human urine sample extracted from the DMA compared to glass. Lastly, in urine samples from an intervention study, more significant ions (145) were identified when using LESA-MS spectra of control and test urine extracted from the DMA. We demonstrate that DMA provides a surface-assisted LESA-MS method delivering significant improvement of the surface extraction repeatability leading to the acquisition of more robust and higher quality data. The DMA shows potential to be used for LESA-MS for controlled and reproducible surface extraction and for acquisition of high quality, qualitative data in a high-throughput manner.
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spelling nottingham-516212020-05-04T19:34:01Z https://eprints.nottingham.ac.uk/51621/ Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning Meurs, Joris Alexander, Morgan R. Levkin, Pavel A. Widmaier, Simon Bunch, Josephine Barrett, David A. Kim, Dong-Hyun A major problem limiting reproducible use of liquid extraction surface analysis (LESA) array sampling of dried surface-deposited liquid samples is the unwanted spread of extraction solvent beyond the dried sample limits, resulting in unreliable data. Here, we explore the use of the Droplet Microarray (DMA), which consists of an array of superhydrophilic spots bordered by a superhydrophobic material giving the potential to confine both the sample spot and the LESA extraction solvent in a defined area. We investigated the DMA method in comparison with a standard glass substrate using LESA analysis of a mixture of biologically relevant compounds with a wide mass range and different physicochemical properties. The optimized DMA method was subsequently applied to urine samples from a human intervention study. Relative standard deviations for the signal intensities were all reduced at least 3-fold when performing LESA-MS on the DMA surface compared with a standard glass surface. Principal component analysis revealed more tight clusters indicating improved spectral reproducibility for a human urine sample extracted from the DMA compared to glass. Lastly, in urine samples from an intervention study, more significant ions (145) were identified when using LESA-MS spectra of control and test urine extracted from the DMA. We demonstrate that DMA provides a surface-assisted LESA-MS method delivering significant improvement of the surface extraction repeatability leading to the acquisition of more robust and higher quality data. The DMA shows potential to be used for LESA-MS for controlled and reproducible surface extraction and for acquisition of high quality, qualitative data in a high-throughput manner. American Chemical Society 2018-04-27 Article PeerReviewed Meurs, Joris, Alexander, Morgan R., Levkin, Pavel A., Widmaier, Simon, Bunch, Josephine, Barrett, David A. and Kim, Dong-Hyun (2018) Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning. Analytical Chemistry, 90 (10). pp. 6001-6005. ISSN 1520-6882 https://pubs.acs.org/doi/10.1021/acs.analchem.8b00973 doi:10.1021/acs.analchem.8b00973 doi:10.1021/acs.analchem.8b00973
spellingShingle Meurs, Joris
Alexander, Morgan R.
Levkin, Pavel A.
Widmaier, Simon
Bunch, Josephine
Barrett, David A.
Kim, Dong-Hyun
Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title_full Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title_fullStr Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title_full_unstemmed Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title_short Improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
title_sort improved extraction repeatability and spectral reproducibility for liquid extraction surface analysis–mass spectrometry using superhydrophobic–superhydrophilic patterning
url https://eprints.nottingham.ac.uk/51621/
https://eprints.nottingham.ac.uk/51621/
https://eprints.nottingham.ac.uk/51621/