SABRE‐enhanced real‐time pure shift NMR spectroscopy

Taylor, Daniel; Natrajan, Louise S.; Nilsson, Mathias; Adams, Ralph W.

doi:10.1002/mrc.5206

Cited by 6 publications

(4 citation statements)

References 39 publications

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“…Numerous hyperpolarization methods were developed to increase the sensitivity of liquid-state NMR by altering nuclear-spin populations at thermal equilibrium. Major developments comprise Overhauser dynamic nuclear polarization (ODNP), − dissolution dynamic nuclear polarization (dDNP), − and parahydrogen-induced polarization (PHIP), − including signal amplification by reversible exchange (SABRE). − …”

Section: Introductionmentioning

confidence: 99%

Selective Isotope Labeling and LC-Photo-CIDNP Enable NMR Spectroscopy at Low-Nanomolar Concentration

Yang

Mickles

et al. 2022

J. Am. Chem. Soc.

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NMR spectroscopy is a powerful tool to investigate molecular structure and dynamics. The poor sensitivity of this technique, however, limits its ability to tackle questions requiring dilute samples. Low-concentration photochemically induced dynamic nuclear polarization (LC-photo-CIDNP) is an optically enhanced NMR technology capable of addressing the above challenge by increasing the detection limit of aromatic amino acids in solution up to 1000-fold, either in isolation or within proteins. Here, we show that the absence of NMR-active nuclei close to a magnetically active site of interest (e.g., the structurally diagnostic 1Hα–13Cα pair of amino acids) is expected to significantly increase LC-photo-CIDNP hyperpolarization. Then, we exploit the spin-diluted tryptophan isotopolog Trp-α-13C-β,β,2,4,5,6,7-d7 and take advantage of the above prediction to experimentally achieve a ca 4-fold enhancement in NMR sensitivity over regular LC-photo-CIDNP. This advance enables the rapid (within seconds) detection of 20 nM concentrations or the molecule of interest, corresponding to a remarkable 3 ng detection limit. Finally, the above Trp isotopolog is amenable to incorporation within proteins and is readily detectable at a 1 μM concentration in complex cell-like media, including Escherichia coli cell-free extracts.

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Section: Introductionmentioning

confidence: 99%

Selective Isotope Labeling and LC-Photo-CIDNP Enable NMR Spectroscopy at Low-Nanomolar Concentration

Yang

Mickles

et al. 2022

J. Am. Chem. Soc.

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“…A pure shift NMR procedure in conjunction with conventional SABRE has been demonstrated recently to a similar effect, as part of a separate strategy to overcome spectral overlap. 37–39…”

Section: Resultsmentioning

confidence: 99%

“…A pure shift NMR procedure in conjunction with conventional SABRE has been demonstrated recently to a similar effect, as part of a separate strategy to overcome spectral overlap. [37][38][39] Operationally, the hyperpolarised spectra acquired here for SABRE-DREAM were achieved through manually repolarising the sample with refreshed p-H 2 after every scan, until an 8-scan phase cycle was complete. The reversibility and reproducibility of the SABRE technique allows this to be possible.…”

Section: Effectiveness Of Sabre-dreammentioning

confidence: 99%

“…Of course, that is not to say that in future studies where more complex hyperpolarised substrates or mixtures are analysed using DREAMTIME that these strategies will not prove useful. A pure shift NMR procedure in conjunction with conventional SABRE has been demonstrated recently to a similar effect, as part of a separate strategy to overcome spectral overlap [37][38][39]. Operationally, the hyperpolarised spectra acquired here for SABRE-DREAM were achieved through manually repolarising the sample with refreshed p-H 2 after every scan, until an 8-scan phase cycle was complete.…”

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confidence: 99%

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Selective NMR detection of individual reaction components hyperpolarised by reversible exchange with para-hydrogen

Norcott

2022

Phys. Chem. Chem. Phys.

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Iridium Pyridylpyrrolides Hyperpolarised by Para‐Hydrogen

Majchrzak,

Norcott

2024

Chemistry A European J

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Chemical activation of the nuclear singlet state of dihydrogen, para‐hydrogen, can dramatically increase the sensitivity of magnetic resonance spectroscopy and imaging. Here, we show that the highly reversible activation of para‐hydrogen by an iridium pyridylpyrrolide complex is capable of producing this hyperpolarisation effect. Bound alkene ligands exhibit signal enhancement without reduction to alkanes, which is in contrast to the most widely used hyperpolarisation catalysts. The complex is recoverable due to the highly reversible binding and release of H2, and result in enhanced hydride signals in a wide range of coordinating and non‐coordinating deuterated solvents. Synthetic modification of the ligand substituents and the addition of co‐ligands show a strong dependence of chemical structure on reactivity, which reveals an untapped potential to exploit pyridylpyrrolides as ligands in the development of tunable para‐hydrogen induced hyperpolarisation catalysts or molecular probes.

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SABRE‐enhanced real‐time pure shift NMR spectroscopy

Cited by 6 publications

References 39 publications

Selective Isotope Labeling and LC-Photo-CIDNP Enable NMR Spectroscopy at Low-Nanomolar Concentration

Selective Isotope Labeling and LC-Photo-CIDNP Enable NMR Spectroscopy at Low-Nanomolar Concentration

Selective NMR detection of individual reaction components hyperpolarised by reversible exchange with para-hydrogen

Iridium Pyridylpyrrolides Hyperpolarised by Para‐Hydrogen

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