Hyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics

Jabadurai Jayapaul, Sanna Komulainen, Vladimir V. Zhivonitko, Jiří Mareš, Chandan Giri, Kari Rissanen, Perttu Lantto (), Ville-Veikko Telkki and Leif Schröder ()
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Jabadurai Jayapaul: Leibniz-Forschungsinstitut für Molekulare Pharmakologie (FMP)
Sanna Komulainen: NMR Research Unit, University of Oulu
Vladimir V. Zhivonitko: NMR Research Unit, University of Oulu
Jiří Mareš: NMR Research Unit, University of Oulu
Chandan Giri: University of Jyvaskyla, Department of Chemistry
Kari Rissanen: University of Jyvaskyla, Department of Chemistry
Perttu Lantto: NMR Research Unit, University of Oulu
Ville-Veikko Telkki: NMR Research Unit, University of Oulu
Leif Schröder: Leibniz-Forschungsinstitut für Molekulare Pharmakologie (FMP)

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Guest capture and release are important properties of self-assembling nanostructures. Over time, a significant fraction of guests might engage in short-lived states with different symmetry and stereoselectivity and transit frequently between multiple environments, thereby escaping common spectroscopy techniques. Here, we investigate the cavity of an iron-based metal organic polyhedron (Fe-MOP) using spin-hyperpolarized 129Xe Chemical Exchange Saturation Transfer (hyper-CEST) NMR. We report strong signals unknown from previous studies that persist under different perturbations. On-the-fly delivery of hyperpolarized gas yields CEST signatures that reflect different Xe exchange kinetics from multiple environments. Dilute pools with ~ 104-fold lower spin numbers than reported for directly detected hyperpolarized nuclei are readily detected due to efficient guest turnover. The system is further probed by instantaneous and medium timescale perturbations. Computational modeling indicates that these signals originate likely from Xe bound to three Fe-MOP diastereomers (T, C3, S4). The symmetry thus induces steric effects with aperture size changes that tunes selective spin manipulation as it is employed in CEST MRI agents and, potentially, impacts other processes occurring on the millisecond time scale.

Date: 2022
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DOI: 10.1038/s41467-022-29249-w

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