An Ultrahigh CO2-Loaded Silicalite-1 Zeolite: Structural Stability and Physical Properties at High Pressures and Temperatures

Tomas Marqueno, David Santamaria-Perez*, Javier Ruiz-Fuertes, Raquel Chulia-Jordan, Jose L. Jorda, Fernando Rey, Chris McGuire, Abby Kavner, Simon MacLeod, Dominik Daisenberger, Catalin Popescu, Placida Rodriguez-Hernandez, Alfonso Munoz

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

We report the formation of an ultrahigh CO2-loaded pure-SiO2, silicalite-1 structure at high pressure (0.7 GPa) from the interaction of empty zeolite and fluid CO, medium. The CO2-filled structure was characterized in situ by means of synchrotron powder X-ray diffraction. Rietveld refinements and Fourier recycling allowed the location of 16 guest carbon dioxide molecules per unit cell within the straight and sinusoidal channels of the porous framework to be analyzed. The complete filling of pores by CO, molecules favors structural stability under compression, avoiding pressure-induced amorphization below 20 GPa, and significantly reduces the compressibility of the system compared to that of the parental empty one. The structure of CO2-loaded silicalite-1 was also monitored at high pressures and temperatures, and its thermal expansivity was estimated.

Original languageEnglish
Pages (from-to)6447-6455
Number of pages9
JournalInorganic Chemistry
Volume57
Issue number11
Early online date8 May 2018
DOIs
Publication statusPublished - 4 Jun 2018

Keywords

  • INITIO MOLECULAR-DYNAMICS
  • TOTAL-ENERGY CALCULATIONS
  • POWDER DIFFRACTION
  • CARBON-DIOXIDE
  • CO2
  • ADSORPTION
  • BEHAVIOR
  • METALS
  • TRANSITION
  • SIMULATION

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