TY - JOUR
T1 - An Ultrahigh CO2-Loaded Silicalite-1 Zeolite
T2 - Structural Stability and Physical Properties at High Pressures and Temperatures
AU - Marqueno, Tomas
AU - Santamaria-Perez, David
AU - Ruiz-Fuertes, Javier
AU - Chulia-Jordan, Raquel
AU - Jorda, Jose L.
AU - Rey, Fernando
AU - McGuire, Chris
AU - Kavner, Abby
AU - MacLeod, Simon
AU - Daisenberger, Dominik
AU - Popescu, Catalin
AU - Rodriguez-Hernandez, Placida
AU - Munoz, Alfonso
PY - 2018/6/4
Y1 - 2018/6/4
N2 - 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.
AB - 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.
KW - INITIO MOLECULAR-DYNAMICS
KW - TOTAL-ENERGY CALCULATIONS
KW - POWDER DIFFRACTION
KW - CARBON-DIOXIDE
KW - CO2
KW - ADSORPTION
KW - BEHAVIOR
KW - METALS
KW - TRANSITION
KW - SIMULATION
U2 - 10.1021/acs.inorgchem.8b00523
DO - 10.1021/acs.inorgchem.8b00523
M3 - Article
VL - 57
SP - 6447
EP - 6455
JO - Inorganic Chemistry
JF - Inorganic Chemistry
SN - 0020-1669
IS - 11
ER -