Analysis of urine, oral fluid and fingerprints by liquid extraction surface analysis coupled to high resolution MS and MS/MS – opportunities for forensic and biomedical science

Bailey, Melanie J.; Randall, Elizabeth C.; Costa, Catia; Salter, Tara L.; Race, Alan; Puit, Marcel de; Koeberg, Mattijs; Baumert, Mark; Bunch, Josephine

doi:10.1039/c6ay00782a

Cited by 40 publications

(39 citation statements)

References 39 publications

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“…Although LESA mass spectrometry has been widely applied to the analysis of small molecules (eg, drugs and their metabolites), comparatively few reports describe intact protein analysis from tissue. Schey et al applied manual LESA extraction to sections of bovine ocular lens and mouse brain and kidney.…”

Section: Ambient In Situ Analysis Of Intact Proteins In Biological Sumentioning

confidence: 99%

Ambient ionisation mass spectrometry for in situ analysis of intact proteins

2018

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Ambient surface mass spectrometry is an emerging field which shows great promise for the analysis of biomolecules directly from their biological substrate. In this article, we describe ambient ionisation mass spectrometry techniques for the in situ analysis of intact proteins. As a broad approach, the analysis of intact proteins offers unique advantages for the determination of primary sequence variations and posttranslational modifications, as well as interrogation of tertiary and quaternary structure and protein‐protein/ligand interactions. In situ analysis of intact proteins offers the potential to couple these advantages with information relating to their biological environment, for example, their spatial distributions within healthy and diseased tissues. Here, we describe the techniques most commonly applied to in situ protein analysis (liquid extraction surface analysis, continuous flow liquid microjunction surface sampling, nano desorption electrospray ionisation, and desorption electrospray ionisation), their advantages, and limitations and describe their applications to date. We also discuss the incorporation of ion mobility spectrometry techniques (high field asymmetric waveform ion mobility spectrometry and travelling wave ion mobility spectrometry) into ambient workflows. Finally, future directions for the field are discussed.

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Section: Ambient In Situ Analysis Of Intact Proteins In Biological Sumentioning

confidence: 99%

Ambient ionisation mass spectrometry for in situ analysis of intact proteins

2018

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“…A LESA extraction solvent was prepared containing methanol, water, and formic acid in a volume ratio of, respectively, 70:30:0.1. 3 Slides were placed onto the LESA universal plate holder and scanned with an Epson V300 scanner, and coordinates of sample locations were selected with LESA Points software (Advion Biosciences, Inc., Ithaca, USA). After that, LESA was performed using the TriVersa Nanomate (Advion Biosciences, Inc., Ithaca, USA).…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…L iquid extraction surface analysis−mass spectrometry (LESA-MS) is an ambient mass spectrometry technique in which analytes are extracted from a surface by the formation of a liquid microjunction between the extraction solvent and the surface. 1 This technique has already been widely applied for the analysis of proteins, 2 metabolites, 3 drugs, 3 and lipids 4 in a wide range of matrices and on various surface substrates. One of the main limitations of LESA-MS is poor repetitive sampling due to spreading of the probe solvent on the surface of interest.…”

Section: * S Supporting Informationmentioning

confidence: 99%

Improved Extraction Repeatability and Spectral Reproducibility for Liquid Extraction Surface Analysis–Mass Spectrometry Using Superhydrophobic–Superhydrophilic Patterning

et al. 2018

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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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“…Its ease of use, reproducibility, automated functionality, and ability to interrogate discrete regions of a sample have been demonstrated for the analysis of several classes of biomolecules from a range of surfaces, including tissue, dried blood spots, food surfaces, and latent fingerprints . Previous studies have shown the capabilities and application of LESA, which utilized disposable capillary tips and enabled offline proteomics analysis of tissue extracts . Recently, this liquid extraction technology has been modified by replacing the disposable capillary with a glass capillary (LESAplus) allowing for increased droplet resolution on the sample surface.…”

Section: Introductionmentioning

confidence: 99%