Hyperpolarization-Enhanced NMR Spectroscopy of Unaltered Biofluids Using Photo-CIDNP
Kuhn, Lars T. (Albert-Ludwigs-Universität Freiburg. Institut für Physikalische Chemie)
Weber, Stefan (Albert-Ludwigs-Universität Freiburg. Institut für Physikalische Chemie)
Bargon, Joachim (Rheinische Friedrich-Wilhelms-Universität Bonn. Institut für Physikalische und Theoretische Chemie)
Parella Coll, Teodor (Universitat Autònoma de Barcelona. Servei de Ressonància Magnètica Nuclear)
Pérez-Trujillo, Míriam (Universitat Autònoma de Barcelona. Servei de Ressonància Magnètica Nuclear)
Data: |
2024 |
Resum: |
The direct and unambiguous detection and identification of individual metabolite molecules present in complex biological mixtures constitute a major challenge in (bio)analytical research. In this context, nuclear magnetic resonance (NMR) spectroscopy has proven to be particularly powerful owing to its ability to provide both qualitative and quantitative atomic-level information on multiple analytes simultaneously in a noninvasive manner. Nevertheless, NMR suffers from a low inherent sensitivity and, moreover, lacks selectivity regarding the number of individual analytes to be studied in a mixture of a myriad of structurally and chemically very different molecules, e. g. , metabolites in a biofluid. Here, we describe a method that circumvents these shortcomings via performing selective, photochemically induced dynamic nuclear polarization (photo-CIDNP) enhanced NMR spectroscopy on unmodified complex biological mixtures, i. e. , human urine and serum, which yields a single, background-free one-dimensional NMR spectrum. In doing this, we demonstrate that photo-CIDNP experiments on unmodified complex mixtures of biological origin are feasible, can be performed straightforwardly in the native aqueous medium at physiological metabolite concentrations, and act as a spectral filter, facilitating the analysis of NMR spectra of complex biofluids. Due to its noninvasive nature, the method is fully compatible with state-of-the-art metabolomic protocols providing direct spectroscopic information on a small, carefully selected subset of clinically relevant metabolites. We anticipate that this approach, which, in addition, can be combined with existing high-throughput/high-sensitivity NMR methodology, holds great promise for further in-depth studies and development for use in metabolomics and many other areas of analytical research. |
Ajuts: |
Agencia Estatal de Investigación PGC2018-095808-B-I00
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Nota: |
Altres ajuts: acords transformatius de la UAB |
Drets: |
Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original. |
Llengua: |
Anglès |
Document: |
Article ; recerca ; Versió publicada |
Matèria: |
Analytical research ;
Biofluids ;
Biological mixtures ;
Detection and identifications ;
Dynamic nuclear polarization ;
Hyperpolarization ;
Identification of individuals ;
Magnetic resonance spectra ;
Metabolomics ;
Photo-CIDNP |
Publicat a: |
Analytical chemistry, Vol. 96, Issue 1 (September 2024) , p. 102-109, ISSN 1520-6882 |
DOI: 10.1021/acs.analchem.3c03215
PMID: 38109875
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Registre creat el 2024-01-24, darrera modificació el 2024-05-06