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Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support

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    Charge Transfer Stabilization of Late Transition Metal Oxide Nanoparticles on a Layered Niobate Support
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    † †Departments of Chemistry, Physics, and Biochemistry and Molecular Biology and ‡Department of Chemical Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States
    § Center for Nanoscale Science and Technology, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States
    *[email protected]
    *[email protected]
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2015, 137, 51, 16216–16224
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    https://doi.org/10.1021/jacs.5b11230
    Published December 10, 2015
    Copyright © 2015 American Chemical Society
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    Abstract

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    Interfacial interactions between late transition metal/metal oxide nanoparticles and oxide supports impact catalytic activity and stability. Here, we report the use of isothermal titration calorimetry (ITC), electron microscopy and density functional theory (DFT) to explore periodic trends in the heats of nanoparticle–support interactions for late transition metal and metal oxide nanoparticles on layered niobate and silicate supports. Data for Co(OH)2, hydroxyiridate-capped IrOx·nH2O, Ni(OH)2, CuO, and Ag2O nanoparticles were added to previously reported data for Rh(OH)3 grown on nanosheets of TBA0.24H0.76Ca2Nb3O10 and a layered silicate. ITC measurements showed stronger bonding energies in the order Ag < Cu ≈ Ni ≈ Co < Rh < Ir on the niobate support, as expected from trends in M–O bond energies. Nanoparticles with exothermic heats of interaction were stabilized against sintering. In contrast, ITC measurements showed endothermic interactions of Cu, Ni, and Rh oxide/hydroxide nanoparticles with the silicate and poor resistance to sintering. These trends in interfacial energies were corroborated by DFT calculations using single-atom and four-atom cluster models of metal/metal oxide nanoparticles. Density of states and charge density difference calculations reveal that strongly bonded metals (Rh, Ir) transfer d-electron density from the adsorbed cluster to niobium atoms in the support; this mixing is absent in weakly binding metals, such as Ag and Au, and in all metals on the layered silicate support. The large differences between the behavior of nanoparticles on niobate and silicate supports highlight the importance of d-orbital interactions between the nanoparticle and support in controlling the nanoparticles’ stability.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.5b11230.

    • Details of obtaining thermochemical data from ITC experiments, XRD of bulk nanoparticles and nanoparticle/support composites, TEM and UV–vis of hydroxyiridate-capped IrOx·nH2O particles, sintering studies of supported metal oxide nanoparticles, surface models used for DFT binding energy calculations, optimized single atom and metal cluster adsorption geometries, charge density difference plots, list of nanoparticles and metal precursors, and heats of formation of oxides and sublimation of metals (17 pp). (PDF)

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    Cite this: J. Am. Chem. Soc. 2015, 137, 51, 16216–16224
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    https://doi.org/10.1021/jacs.5b11230
    Published December 10, 2015
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