[논문]Alumina-supported bimetallics of palladium alloyed with germanium, tin, lead, or antimony from organometallic precursors II. gas-phase hydrogenation of 2-methyl-1-buten-3-yne (valylene) and 2-methyl-1,3-butadiene (isoprene)

doi:10.1016/0021-9517(91)90008-R

Alumina-supported bimetallics of palladium alloyed with germanium, tin, lead, or antimony from organometallic precursors II. gas-phase hydrogenation of 2-methyl-1-buten-3-yne (valylene) and 2-methyl-1,3-butadiene (isoprene)

Journal of catalysis, v.129 no.1, 1991년, pp.47 - 57

Aduriz, Hugo R. (Laboratoire de Chimie Organique Physique et Ciné) , Bodnariuk, Pedro (tique Chimique Appliqué) , Coq, Bernard (es, UA 418 du CNRS, ENSCM, 8, Rue de L'Ecole Normale, 34053 Montpellier Cedex, France) , Figueras, François (Laboratoire de Chimie Organique Physique et Ciné)

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Abstract A series of PdGe, PdSb, PdSn, and PdPb/α-Al2O3 catalysts, prepared by the controlled surface reaction (CSR) technique from organometallic precursors have been tested in the gas-phase hydrogenation of 2-methyl-1-buten-3-yne (valylene) and 2-methyl-1,3-butadiene (isoprene). On catalysts reduced at 573 K, the turnover frequencies for valylene (TONV) and isoprene (TONI) hydrogenation were not modified by addition to the 0.09 wt% Pd/α-Al2O3 base catalyst of Ge, Sb, Sn, or Pb, up to 0.1 wt% (at 293 K: TONV = 20 s−1 and TONI = 33 s−1). Pd/α-Al2O3 reduced at 773 K was severely sintered (dTEM increased from 2.8 run to 12.4 nm) and TONV and TONI at 293 K increased to 190 and 283 s−1, respectively, as a result of an apparent crystal size effect: the reactants adsorb more strongly on the smaller Pd particles. Upon alloying with Ge, Sb, Sn, or Pb and a subsequent reduction at 773 K, a modest decrease of both TONV (by a factor of 2) and TONI (by a factor of 2–5) was observed. At high conversion, both the selectivity to isoprene (SI) in valylene hydrogenation, and to olefins (SO) in isoprene hydrogenation on Pd/α-Al2O3 were improved upon alloying with Sb, Sn, or Pb (Ge had no effect). In addition, the isomerization of 2-methyl-1-butene and 3-methyl-1-butene (double bond migration reaction) during isoprene hydrogenation was partially suppressed on PdSn and PdPb/α-Al2O3. The improvement in selectivities was interpreted in terms of a change in the relative adsorption strength of the reactants and intermediate products over the new bimetallic sites.

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Alumina-supported bimetallics of palladium alloyed with germanium, tin, lead, or antimony from organometallic precursors II. gas-phase hydrogenation of 2-methyl-1-buten-3-yne (valylene) and 2-methyl-1,3-butadiene (isoprene)

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