A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Encapsulation of xenon by bridged resorcinarene cages with high 129Xe NMR chemical shift and efficient exchange dynamics (2023)
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
JYU-tekijät tai -toimittajat
Julkaisun tiedot
Julkaisun kaikki tekijät tai toimittajat: Komulainen, Sanna; Iresh Fernando, P. U. Ashvin; Mareš, Jiří; Selent, Anne; Khalili, Roya; Cesana, Paul T.; Ebeling, Andreas; Kantola, Anu M.; Beyeh, Ngong Kodiah; Rissanen, Kari; et al.
Lehti tai sarja: Cell Reports Physical Science
eISSN: 2666-3864
Julkaisuvuosi: 2023
Ilmestymispäivä: 08.02.2023
Volyymi: 4
Lehden numero: 2
Artikkelinumero: 101281
Kustantaja: Elsevier
Julkaisumaa: Yhdysvallat (USA)
Julkaisun kieli: englanti
DOI: https://doi.org/10.1016/j.xcrp.2023.101281
Julkaisun avoin saatavuus: Avoimesti saatavilla
Julkaisukanavan avoin saatavuus: Kokonaan avoin julkaisukanava
Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/85668
Tiivistelmä
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).
YSO-asiasanat: supramolekulaarinen kemia; biosensorit; ksenon; molekyylidynamiikka; laskennallinen kemia
Vapaat asiasanat: supermolecules; functionalized cages; biosensors; piperazine-bridged resorcinarenes; aliphatically bridged resorcinarenes; 129Xe NMR; 129Xe HyperCEST MRI; first principal modeling; molecular dynamic simulations
Liittyvät organisaatiot
OKM-raportointi: Kyllä
VIRTA-lähetysvuosi: 2023
JUFO-taso: 1
