4.8 Article

Inside information on xenon adsorption in porous organic cages by NMR

Journal

CHEMICAL SCIENCE
Volume 8, Issue 8, Pages 5721-5727

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c7sc01990d

Keywords

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Funding

  1. Academy of Finland [289649, 294027, 285666]
  2. Engineering and Physical Sciences Research Council (EPSRC) [EP/H000925/1, EP/N004884/1]
  3. European Research Council under the European Union's Seventh Framework Programme (FP)/ERC [321156]
  4. Royal Society
  5. EPSRC [EP/N004884/1, EP/H000925/1, EP/K039687/1] Funding Source: UKRI
  6. Engineering and Physical Sciences Research Council [EP/N004884/1, EP/K039687/1, EP/H000925/1] Funding Source: researchfish

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A solid porous molecular crystal formed from an organic cage, CC3, has unprecedented performance for the separation of rare gases. Here, xenon was used as an internal reporter providing extraordinarily versatile information about the gas adsorption phenomena in the cage and window cavities of the material. Xe-129 NMR measurements combined with state-of-the-art quantum chemical calculations allowed the determination of the occupancies of the cavities, binding constants, thermodynamic parameters as well as the exchange rates of Xe between the cavities. Chemical exchange saturation transfer (CEST) experiments revealed a minor window cavity site with a significantly lower exchange rate than other sites. Diffusion measurements showed significantly reduced mobility of xenon with loading. Xe-129 spectra also revealed that the cage cavity sites are preferred at lower loading levels, due to more favourable binding, whereas window sites come to dominate closer to saturation because of their greater prevalence.

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