| Zugriffsnummer | 48097 |
| Dokumenttyp | Zeitschriftenartikel |
| Peer Review | mit Peer Review |
| Sprache | Englisch |
| Titel | Comprehensive quantitative and calibration-free evaluation of hyperpolarized xenon-host interaction by multiparametric NMR |
| Autor(in); Institution |
Korchak, Sergey; 8.1, Biomedizinische Magnetresonanz, PTB-Berlin; MPI Multidisciplinary Sciences, Göttingen, GERMANY
Kilian, Wolfgang; 8.1, Biomedizinische Magnetresonanz, PTB-Berlin
Riemer, Thomas; 8.3, Biomedizinische Optik, PTB-Berlin; TU Leipzig, GERMANY
|
| Quelle/Jahr | Analytical Chemistry: 94 (2022), 2561 - 2568 |
| ISSN | 0096-4484 (PRINT) ; 1520-6882 (ONLINE) |
| DOI | |
| Verlag | Washington, DC: ACS Publications |
| Zusammenfassung | The probing of microscopic environments by hyperpolarized xenon NMR has spurred investigations in supramolecular chemistry as well as important biosensing and molecular imaging applications. While xenon exchange with host structures at micro-molar concentration and below can be readily detected, quantitative analysis is limited, requiring complementary experimentation by different methodologies, lacking completeness and compromising validity and comparability of numerical results. Here, a new NMR measurement and data analysis approach is introduced for the comprehensive characterization of the host-xenon binding dynamics. Application of chemical exchange saturation transfer of hyperpolarized 129Xe under parametric modulation of the saturation RF amplitude and xenon gas saturation of the solution enables delineation of exchange mechanisms and, through modeling, numerical estimation of the various rate coefficients (and thus exchange rates), the xenon affinity, and the total host molecule concentration. Only the numerical xenon solubility is additionally required for input, a quantity of low impact on the measurement uncertainty and derivable from metrological data collections. Signal calibration by reference material may thus be avoided, qualifying the method as calibration-free. For demonstration the xenon exchange with the small host cucurbit[6]uril at low concentration is investigated with the numerical results validated by comparison with standard quantitative NMR data obtained at high host concentration. The readiness to evaluate xenon exchange for the one sample at hand and in a single experimental attempt by the proposed method may allow comprehensive quantitative studies in supramolecular chemistry, bio-macromolecular structure and dynamics, and sensing. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.1c04482. |
| Themenbereich der Metrologie | Metrologie in der Medizin |