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Isotope-selective pore opening in a flexible metal-organic framework.

Linda BondorfJhonatan Luiz FiorioVolodymyr BonLinda ZhangMariia MaliutaSebastian EhrlingIrena SenkovskaJack D EvansJan-Ole JoswigStefan KaskelThomas HeineMichael Hirscher
Published in: Science advances (2022)
Flexible metal-organic frameworks that show reversible guest-induced phase transitions between closed and open pore phases have enormous potential for highly selective, energy-efficient gas separations. Here, we present the gate-opening process of DUT-8(Ni) that selectively responds to D 2 , whereas no response is observed for H 2 and HD. In situ neutron diffraction directly reveals this pressure-dependent phase transition. Low-temperature thermal desorption spectroscopy measurements indicate an outstanding D 2 -over-H 2 selectivity of 11.6 at 23.3 K, with high D 2 uptake. First-principles calculations coupled with statistical thermodynamics predict the isotope-selective gate opening, rationalized by pronounced nuclear quantum effects. Simulations suggest DUT-8(Ni) to remain closed in the presence of HT, while it also opens for DT and T 2 , demonstrating gate opening as a highly effective approach for isotopolog separation.
Keyphrases
  • metal organic framework
  • molecular dynamics
  • monte carlo
  • solid state
  • minimally invasive
  • single molecule
  • molecular dynamics simulations
  • gas chromatography
  • mass spectrometry
  • risk assessment
  • ionic liquid