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Water-Soluble Pyrene Tags Enable the Detection of Carbohydrates by Label-Assisted Laser Desorption/ionisation Mass Spectrometry

preprint
revised on 30.06.2020, 16:53 and posted on 01.07.2020, 13:06 by Jacob R Hauser, Edmund T Bergström, Alexander N. Kulak, Stuart L Warriner, Jane E Thomas-Oates, Robin Bon
Matrix-assisted laser desorption/ionisation mass spectrometry (MALDI-MS) is widely used for the analysis of biomolecules. Label-assisted laser desorption/ionisation mass spectrometry (LALDI-MS) is a matrix-free variant of MALDI-MS, in which only analytes covalently attached to a laser desorption/ionisation (LDI) enhancer are detected. LALDI-MS has shown promise in overcoming limitations of MALDI-MS in terms of sample preparation and MS analysis. In this work, we have developed water-soluble pyrene-based LDI reagents (LALDI tags) that can be used for (in situ) labelling and LALDI-MS analysis of reducing carbohydrates from complex (biological) samples without the need for additional chemical derivatisation or purification. We have systematically explored the suitability of four pyrene-based LDI enhancers and three aldehyde-reactive handles, optimised sample preparation, and exemplified the use of a LALDI tag by the detection of lactose in cow’s milk. These results demonstrate that LALDI-MS is a promising technique for the analysis of reducing carbohydrates in biological samples, and pave the way for the development of LALDI-MS for glycomics and diagnostics.

Funding

Core Capability for Chemistry Research - Leeds

Engineering and Physical Sciences Research Council

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Core Capability - University of York

Engineering and Physical Sciences Research Council

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Technologies for the Future

Engineering and Physical Sciences Research Council

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Yorkshire Forward (funds from the Northern Way Initiative)

History

Email Address of Submitting Author

r.bon@leeds.ac.uk

Institution

University of Leeds

Country

UK

ORCID For Submitting Author

0000-0003-1733-3680

Declaration of Conflict of Interest

The authors declare no conflict of interest

Version Notes

ChemRxiv Version 2 (references 11 and 22 corrected)

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