title: Supported molecular iridium catalysts: resolving effects of metal nuclearity and supports as ligands.
abstract: The performance of a supported catalyst is influenced by the size and structure of the metal species, the ligands bonded to the metal, and the support. Resolution of these effects has been lacking because of the lack of investigations of catalysts with uniform and systematically varied catalytic sites. We now demonstrate that the performance for ethene hydrogenation of isostructural iridium species on supports with contrasting properties as ligands (electron-donating MgO and electron-withdrawing HY zeolite) can be elucidated on the basis of molecular concepts. Spectra of the working catalysts show that the catalytic reaction rate is determined by the dissociation of H(2) when the iridium, either as mono- or tetra-nuclear species, is supported on MgO and is not when the support is the zeolite. The neighboring iridium sites in clusters are crucial for activation of both H(2) and C(2)H(4) when the support is MgO but not when it is the zeolite, because the electron-withdrawing properties of the zeolite support enable even single site-isolated Ir atoms to bond to both C(2)H(4) and H(2) and facilitate the catalysis.
authors.affiliation: Department of Chemical Engineering and Materials Science, University of California-Davis, One Shields Avenue, Davis, California 95616, United States.
authors.forename: Jing
authors.initials: J
authors.lastname: Lu
authors.forename: Pedro
authors.initials: P
authors.lastname: Serna
authors.forename: Ceren
authors.initials: C
authors.lastname: Aydin
authors.forename: Nigel D
authors.initials: ND
authors.lastname: Browning
authors.forename: Bruce C
authors.initials: BC
authors.lastname: Gates