García Ricard, Omar J.

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    Pillar-layered structured nanoporous coordination polymers for carbon dioxide adsorption-based applications
    (2013) García Ricard, Omar J.; Hernández Maldonado, Arturo J.; College of Engineering; Curet Arana, María C.; Martínez Iñesta, María M.; Cardona Martínez, Nelson; Department of Chemical Engineering; Papadopoulos, Christopher
    Porous coordination polymers (PCPs) have been of great interest for scientist and engineers due to their potential use in applications such as heterogeneous catalysis, molecular storage, and gas separation via adsorption. In this work, a series of PCPs with a coordination pillar-layered structure in which different organic pillar ligands can be used to obtain isostructural adsorbents with different pore sizes and functionalities, the so-called CPL-n series, was studied. The textural, structural, and adsorption properties of various adsorbents within the CPL-n series were evaluated for different activation temperatures, where a decrease in surface area and pore volume was observed for activation temperatures well below the decomposition limit of the materials. To understand the effect of the activation temperature on CPL-n textural properties, various material characterization techniques were employed. In situ high-temperature and high-vacuum infrared spectroscopy and differential scanning calorimetry coupled with X-ray diffraction (DSC-XRD) showed the desorption of water molecules with no long-range structural or phase changes for the different activation temperatures, that may explain the change in textural properties. In situ high-temperature solid-state Nuclear Magnetic Resonance (NMR) was used to observe the unbinding of the pillar ligands from the coordination center that were effectively blocking the micropores and decreasing the measured surface area and volume. This phenomenon also affected the CPL-n gas adsorption performance, as a decrease in the carbon dioxide adsorption capacity was also noted for the higher activation temperatures. As all the CPL-n series showed higher selectivity for carbon dioxide over other light gases like methane and nitrogen, two CPLs were evaluated for the short-term gas storage and delivery in portable closed-volume applications, where they both showed superior performance when compared to a commercial PCP. The functionalization with metal cations in two CPLs is also presented, where sodium cations were incorporated in their micropores, resulting in a change in the shape of the isotherm with enhanced adsorption capacity in the low partial pressure range.