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Hydrogenation of ethylene over palladium: evolution of the catalyst structure by operando synchrotron-based techniques.
Bugaev, Aram L; Usoltsev, Oleg A; Guda, Alexander A; Lomachenko, Kirill A; Brunelli, Michela; Groppo, Elena; Pellegrini, Riccardo; Soldatov, Alexander V; van Bokhoven, Jeroen A.
Afiliação
  • Bugaev AL; The Smart Materials Research Institute, Southern Federal University, Sladkova 178/24, Rostov-on-Don, 344090, Russia. abugaev@sfedu.ru.
  • Usoltsev OA; The Smart Materials Research Institute, Southern Federal University, Sladkova 178/24, Rostov-on-Don, 344090, Russia. abugaev@sfedu.ru.
  • Guda AA; The Smart Materials Research Institute, Southern Federal University, Sladkova 178/24, Rostov-on-Don, 344090, Russia. abugaev@sfedu.ru.
  • Lomachenko KA; BM23/ID24, European Synchrotron Radiation Facility, 71 avenue des Martyrs, 38043 Grenoble Cedex 9, France.
  • Brunelli M; DUBBLE CRG at the European Synchrotron Radiation Facility, Netherlands Organization for Scientific Research (NWO), 71 Avenue des Martyrs, 38042 Grenoble Cedex 9, France.
  • Groppo E; Department of Chemistry, NIS Interdepartmental Centre, University of Turin, via P. Giuria 7, 10125 Turin, Italy.
  • Pellegrini R; Chimet S.p.A. - Catalyst Division, Via di Pescaiola 74, 52041 Viciomaggio Arezzo, Italy.
  • Soldatov AV; The Smart Materials Research Institute, Southern Federal University, Sladkova 178/24, Rostov-on-Don, 344090, Russia. abugaev@sfedu.ru.
  • van Bokhoven JA; Institute for Chemical and Bioengineering, ETH Zurich, Vladimir-Prelog-Weg 1, 8093 Zurich, Switzerland and Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
Faraday Discuss ; 229: 197-207, 2021 May 01.
Article em En | MEDLINE | ID: mdl-33656030
ABSTRACT
Palladium-based catalysts are exploited on an industrial scale for the selective hydrogenation of hydrocarbons. The formation of palladium carbide and hydride phases under reaction conditions changes the catalytic properties of the material, which points to the importance of operando characterization for determining the relation between the relative fractions of the two phases and the catalyst performance. We present a combined time-resolved characterization by X-ray absorption spectroscopy (in both near-edge and extended regions) and X-ray diffraction of a working palladium-based catalyst during the hydrogenation of ethylene in a wide range of partial pressures of ethylene and hydrogen. Synergistic coupling of multiple techniques allowed us to follow the structural evolution of the palladium lattice as well as the transitions between the metallic, hydride and carbide phases of palladium. The nanometric dimensions of the particles resulted in the considerable contribution of both surface and bulk carbides to the X-ray absorption spectra. During the reaction, palladium carbide is formed, which does not lead to a loss of activity. Unusual contraction of the unit cell parameter of the palladium lattice in the spent catalyst was observed upon increasing hydrogen partial pressure.

Texto completo: 1 Coleções: 01-internacional Temas: Agentes_cancerigenos Base de dados: MEDLINE Idioma: En Revista: Faraday Discuss Assunto da revista: QUIMICA Ano de publicação: 2021 Tipo de documento: Article País de afiliação: Federação Russa

Texto completo: 1 Coleções: 01-internacional Temas: Agentes_cancerigenos Base de dados: MEDLINE Idioma: En Revista: Faraday Discuss Assunto da revista: QUIMICA Ano de publicação: 2021 Tipo de documento: Article País de afiliação: Federação Russa