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    Two-Step Adsorption of PtCl62- Complexes at a Charged Langmuir Monolayer: Role of Hydration and Ion Correlations

    Year: 2017

    Journal: J. Phys. Chem. C, Volume 121, NOV 16, page 25377–25383

    Authors: Uysal, Ahmet; Rock, William; Qiao, Baofu; Bu, Wei; Lin, Binhua

    Organizations: U.S. Department of Energy, Office of Basic Energy Science, Division of Chemical Sciences, Geosciences, and Biosciences, Heavy Element Chemistry [DE-ACO2-06CH11357]; U.S. Department of Energy, Office of Basic Energy Science [DE-ACO2-06CH11357]; [NSF/CHE-1346572]

    Anion exchange at positively charged interfaces plays an important role in a variety of physical and chemical processes. However, the molecular-scale details of these processes, especially with heavy and large anionic complexes, are not well-understood. We studied the adsorption of PtCl62- anionic complexes to floating DPTAP monolayers in the presence of excess Cl- as a function of the bulk chlorometalate concentration. This system aims to simulate the industrial conditions for heavy metal separations with solvent extraction. In situ X-ray scattering and fluorescence measurements, which are element and depth sensitive, show that the chlorometalate ions only adsorb in the diffuse layer at lower concentrations, while they adsorb predominantly in the Stern layer at higher concentrations. The response of DPTAP molecules to the adsorbed ions is determined independently by grazing incidence X-ray diffraction and supports this picture. Molecular dynamics simulations further elucidate the nanoscale structure of the interfacial complexes. The results suggest that ion hydration and ion-ion correlations play a key role in the competitive adsorption process.
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