DOI

  • Bart Bueken
  • Niels Van Velthoven
  • Tom Willhammar
  • Timothee Stassin
  • Ivo Stassen
  • David A. Keen
  • Gino Baron
  • Joeri Denayer
  • Rob Ameloot
  • Sara Bals
  • Dirk De Vos
  • Thomas Bennett
The ability of metal-organic frameworks (MOFs) to gelate under specific synthetic conditions opens up new opportunities in the preparation and shaping of hierarchically porous MOF monoliths, which could be directly implemented for catalytic and adsorptive applications. In this work, we present the first examples of xero-or aerogel monoliths consisting solely of nanoparticles of several prototypical Zr4+-based MOFs: UiO-66-X (X - H, NH2, NO2, (OH)(2)), UiO-67, MOF-801, MOF-808 and NU-1000. High reactant and water concentrations during synthesis were observed to induce the formation of gels, which were converted to monolithic materials by drying in air or supercritical CO2. Electron microscopy, combined with N-2 physisorption experiments, was used to show that irregular nanoparticle packing leads to pure MOF monoliths with hierarchical pore systems, featuring both intraparticle micropores and interparticle mesopores. Finally, UiO-66 gels were shaped into monolithic spheres of 600 mm diameter using an oil-drop method, creating promising candidates for packed-bed catalytic or adsorptive applications, where hierarchical pore systems can greatly mitigate mass transfer limitations.
Original languageEnglish
Pages (from-to)3939-3948
Number of pages10
JournalChemical Science
Volume8
Issue number5
DOIs
StatePublished - May 2017

    Research areas

  • Temperature Synthesis, Modulated Synthesis, Total Scattering, Thin-Films, Uio-66, Adsorption, Water, Separation, Defects, Nanoparticles

ID: 31692635