Journal
CHEMISTRY OF MATERIALS
Volume 32, Issue 11, Pages 4641-4650Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c01059
Keywords
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Funding
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program [742743]
- Deutsche Forschungsgemeinschaft [FOR 2433]
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The origin of crystal-size-dependent adsorption behavior of flexible metal-organic frameworks is increasingly studied. In this contribution, we probe the solid-fluid interactions of DUT-49 crystals of different size by in situ Xe-129 NMR spectroscopy at 200 K. With decreasing size of the crystals, the average solid-fluid interactions are found to decrease reflected by a decrease in chemical shift of adsorbed xenon from 230 to 200 ppm, explaining the lack of adsorption-induced transitions for smaller crystals. However, recent studies propose that these results can also originate from the presence of lattice defects. To investigate the influence of defects on the adsorption behavior of DUT-49, we synthesized a series of samples with tailored defect concentrations and characterized them by in situ Xe-129 NMR. In comparison to the results obtained for crystals with different size, we find pronounced changes of the adsorption behavior and influence of the chemical shift only for very high concentrations of defects, which further emphasizes the important role of particle size phenomena.
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