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Bugaev, Aram L.; Guda, Alexander A.; Lazzarini, Andrea; Lomachenko, Kirill A.; Groppo, Elena; Pellegrini, Riccardo; Piovano, Andrea; Emerich, Hermann; Soldatov, Alexander V.; Bugaev, Lusegen A.; Dmitriev, Vladimir P.; van Bokhoven, Jeroen A.; Lamberti, Carlo
Catalysis today, 04/2017, Letnik: 283Journal Article
Display omitted •Reversible hydride phase observed in Pd/C catalysts with EXAFS and XRPD.•Irreversible carbide phase observed in Pd/C catalysts with EXAFS and XRPD.•EXAFS and XRPD hardly discriminate Pd-hydrate from Pd-carbide.•XANES simulations easily discriminate Pd-hydrate from Pd-carbide.•The active PdHx (or PdCy) phase can be determined in operando conditions. In a number of hydrogenation reactions, palladium nanoparticles may undergo a transition to the hydride or the carbide phase, which affects the catalytic properties. In the current work, we determine the structural evolution of an industrial Pd/C catalyst in the presence of hydrogen and acetylene by means of in situ X-ray absorption spectroscopy and X-ray powder diffraction. We observe reversible hydride phase formation and irreversible formation of the carbide phase. The near-edge structure of the absorption spectra (XANES) plays the key role in distinguishing between hydride and carbide phases. We show that the presence of hydrogen and carbon atoms have a direct effect on the near-edge region which is reproduced by theoretical simulations performed in the Monte-Carlo approach.
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