Interplay between noble gases and MOFs: Insights from <sup>129</sup>Xe and <sup>83</sup>Kr NMR spectroscopy.
basic_science · Level V
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- Record sourced from PubMed, PMID 41061069.
- Also identified by DOI 10.1126/sciadv.aea1857 and PMC identifier 12506962.
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Abstract
Efficient separation and storage of radioactive noble gas isotopes [krypton-85 (<sup>85</sup>Kr) and xenon-131m/133/135 (<sup>131m/133/135</sup>Xe)] from off-gas during spent nuclear fuel reprocessing are vital for environmental protection and noble gas recovery. Metal-organic frameworks (MOFs) are promising adsorbents, yet atomic-level insights into Xe and Kr adsorption remain limited. Here, we report the first application of high-field solid-state <sup>83</sup>Kr nuclear magnetic resonance (NMR), alongside extensive <sup>129</sup>Xe NMR, to investigate gas adsorption in eight MOFs representing three design strategies: ultramicroporous one-dimensional-channel MOFs with pore sizes matching noble gas diameters, functionalized MOFs, and MOFs with open metal sites. Single-gas and coadsorption studies reveal distinct adsorption sites, guest-host interactions, and gas dynamics in each MOF. Most MOFs retain crystallinity after exposure to 60-kilogray γ radiation. Several radiation-sensitive MOFs exhibit enhanced stability in the presence of Xe, suggesting that Xe adsorption enhances framework stability and may broaden the range of MOFs usable under γ radiation in nuclear off-gas separation. These findings offer valuable molecular-level design insights.