The Atomic Structural Dynamics of γ-Al2O3 Supported Ir–Pt Nanocluster Catalysts Prepared from a Bimetallic Molecular Precursor: A Study Using Aberration-Corrected Electron Microscopy and X-ray Absorption Spectroscopy

Small, Matthew W.; Sanchez, Sergio I.; Menard, Laurent D.; Kang, Joo H.; Frenkel, Anatoly I.; Nuzzo, Ralph G.

doi:10.1021/ja110033g

Title: The Atomic Structural Dynamics of γ-Al₂O₃ Supported Ir–Pt Nanocluster Catalysts Prepared from a Bimetallic Molecular Precursor: A Study Using Aberration-Corrected Electron Microscopy and X-ray Absorption Spectroscopy

Journal Article · Tue Feb 22 00:00:00 EST 2011 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/ja110033g· OSTI ID:1876424

Small, Matthew W. ^[1]; Sanchez, Sergio I. ^[1]; Menard, Laurent D. ^[2]; Kang, Joo H. ^[3]; Frenkel, Anatoly I. ^[4]; Nuzzo, Ralph G. ^[1]

Univ. of Illinois, Urbana, IL (United States)
Univ. of North Carolina, Chapel Hill, NC (United States)
Univ. of Illinois, Urbana, IL (United States); The Dow Chemical Company, Midland, MI (United States)
Yeshiva Univ., New York, NY (United States)

This study describes a prototypical, bimetallic heterogeneous catalyst: compositionally well-defined Ir–Pt nanoclusters with sizes in the range of 1–2 nm supported on γ-Al₂O₃. Deposition of the molecular bimetallic cluster [Ir₃Pt₃(μ-CO)₃(CO)₃(η-C₅Me₅)₃] on γ-Al₂O₃, and its subsequent reduction with hydrogen, provides highly dispersed supported bimetallic Ir–Pt nanoparticles. Using spherical aberration-corrected scanning transmission electron microscopy (Cs-STEM) and theoretical modeling of synchrotron-based X-ray absorption spectroscopy (XAS) measurements, our studies provide unambiguous structural assignments for this model catalytic system. The atomic resolution Cs-STEM images reveal strong and specific lattice-directed strains in the clusters that follow local bonding configurations of the γ-Al₂O₃ support. Combined nanobeam diffraction (NBD) and high-resolution transmission electron microscopy (HRTEM) data suggest the polycrystalline γ-Al₂O₃ support material predominantly exposes (001) and (011) surface planes (ones commensurate with the zone axis orientations frequently exhibited by the bimetallic clusters). Here, the data reveal that the supported bimetallic clusters exhibit complex patterns of structural dynamics, ones evidencing perturbations of an underlying oblate/hemispherical cuboctahedral cluster–core geometry with cores that are enriched in Ir (a result consistent with models based on surface energetics, which favor an ambient cluster termination by Pt) due to the dynamical responses of the M–M bonding to the specifics of the adsorbate and metal–support interactions. Taken together, the data demonstrate that strong temperature-dependent charge-transfer effects occur that are likely mediated variably by the cluster–support, cluster–adsorbate, and intermetallic bonding interactions.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: FG02-07ER46471; FG02-03ER15476; FG02-07ER46453; AC02-06CH11357

OSTI ID:: 1876424

Journal Information:: Journal of the American Chemical Society, Vol. 133, Issue 10; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: The Atomic Structural Dynamics of γ-Al2O3 Supported Ir–Pt Nanocluster Catalysts Prepared from a Bimetallic Molecular Precursor: A Study Using Aberration-Corrected Electron Microscopy and X-ray Absorption Spectroscopy

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Title: The Atomic Structural Dynamics of γ-Al₂O₃ Supported Ir–Pt Nanocluster Catalysts Prepared from a Bimetallic Molecular Precursor: A Study Using Aberration-Corrected Electron Microscopy and X-ray Absorption Spectroscopy