Search NASA⌕ Search

Engineering topics

Benmore, Sophie R.

Publications and source records attributed to Benmore, Sophie R..

A High Energy X-ray Diffraction Study of Amorphous Indomethacin

Amorphous pharmaceuticals often possess a wide range of molecular conformations and bonding arrangements. The x-ray pair distribution function (PDF) method is a powerful technique for the characterization of variations in both intra-molecular and inter-molecular packing arrangements. Here, the x-ray PDF of amorphous Indomethacin is shown to be particularly sensitive to the preferred orientations of the chlorobenzyl ring found in isomers in the crystalline state. In some cases, the chlorobenzyl ring has no preferred torsional angle in the amorphous form, while in others evidence of distinct isomer orientations are observed. Amorphous samples with no preferred torsion angles of the chlorobenzyl ring are found to favor enhanced inter-molecular hydrogen bonding, and this is reflected in the intensity of the first sharp diffraction peak. These significant variations in structure rule out amorphous Indomethacin as a possible standard for x-ray PDF measurements. At high humidity, time resolved PDF's for >40 h reveal water molecules forming hydrogen bonds with Indomethacin molecules. Finally, a simple linear hydrogen bond model indicates that water molecules in the wet amorphous form have similar hydrogen bond strengths to those found between Indomethacin dimers or chains in the dry amorphous form.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Small- and Wide-Angle X-ray Scattering Studies of Liquid–Liquid Phase Separation in Silicate Melts

Incongruent liquid-liquid phase separation is a common phenomenon in molten oxides, but there are few structural studies due to the high temperatures involved ca. >1600oC. In this work, we present a high-energy x-ray combined small/wide angle scattering (SAXS/WAXS) method that can directly probe non-equilibrium phase diagrams. The Porod exponent in the SAXS signal is extracted, which measures the roughness of the interface formed between different phases. Problematic volatilization of silica in Al 2 O 3 -, CaO-, and MgO-bearing silica-rich liquids were minimized using levitation, laser heating and rapid time-resolved measurements (lasting tens of seconds), to probe the kinetics of the phase separation process. The WAXS measurement simultaneously probes the local atomic structure of the liquid state and shows that the primary structural changes are associated with the SiO 2 network. Cation coordination numbers extracted from pair distribution functions support the model that the origin of phase separation in binary silicate systems is due to Coulombic repulsions between poorly screened cations. For CaO-SiO 2 , the liquid-liquid phase separation is found to correlate with a pause in the temperature dependent atomic disorder associated with SiO4 tetrahedra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗