Encapsulation of xenon by bridged resorcinarene cages with high 129Xe NMR chemical shift and efficient exchange dynamics
Komulainen, S., Iresh Fernando, P. U. A., Mareš, J., Selent, A., Khalili, R., Cesana, P. T., Ebeling, A., Kantola, A. M., Beyeh, N. K., Rissanen, K., DeBoef, B., Lantto, P., & Telkki, V.-V. (2023). Encapsulation of xenon by bridged resorcinarene cages with high 129Xe NMR chemical shift and efficient exchange dynamics. Cell Reports Physical Science, 4(2), Article 101281. https://doi.org/10.1016/j.xcrp.2023.101281
Published inCell Reports Physical Science
DisciplineOrgaaninen kemiaOrganic Chemistry
© 2023 The Author(s)
Functionalized cages encapsulating xenon atoms enable highly sensitive, background-free molecular imaging through a technique known as HyperCEST 129Xe MRI. Here, we introduce a class of potential biosensor cage structures based on two resorcinarene macrocycles bridged either by aliphatic carbon chains or piperazines. First-principles-based modeling predicts a high chemical shift (about 345 ppm) outside the typical experimental observation window for 129Xe encapsulated by the aliphatically bridged cage and two 129Xe resonances for the piperazine-bridged cages corresponding to single and double loading. Based on the computational predictions as well as 129Xe chemical exchange saturation transfer (CEST) and T2 relaxation nuclear magnetic resonance experiments, we confirm Xe encapsulation in the aliphatically bridged and double encapsulation in the piperazine-bridged resorcinarene in methanol. The cages show fast Xe exchange rates (12,000–49,000 s−1), resulting in a high CEST response regardless of the relatively low binding constant (0.09–3 M−1). ...
ISSN Search the Publication Forum2666-3864
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Additional information about fundingFinancial support from the European Research Council (Project number 772110), Academy of Finland (grant no. 340099), and the University of Oulu (Kvantum Institute) is gratefully acknowledged. Part of the work was carried out with the support of the Center for Material Analysis, University of Oulu, Finland. Computational resources of CSC (Espoo, Finland) and the Finnish Grid and Cloud Infrastructure project (persistent identifier urn:nbn:fi:research-infras-2016072533) were used. American Chemical Society (N.K.B.: ACS-PRF grant no. 39427) and Oakland University, MI, USA, are acknowledged. ...
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