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Klanjšek, M.; Gradišek, A.; Kocjan, A.; Bobnar, M.; Jeglič, P.; Wencka, M.; Jagličić, Z.; Popčević, Petar; Ivkov, Jovica; Smontara, Ana; Gille, Peter; Armbrüster, Marc; Grin, Yuri und Dolinšek, Janez (2012): PdGa intermetallic hydrogenation catalyst: An NMR and physical property study. In: Journal of Physics Condensed Matter, Bd. 24, Nr. 8

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Abstract

The PdGa intermetallic compound is a highly selective and stable heterogeneous hydrogenation catalyst for the semi-hydrogenation of acetylene. We have studied single crystals of PdGa grown by the Czochralski technique. The 69Ga electric-field-gradient (EFG) tensor was determined by means of NMR spectroscopy, giving experimental confirmation of both the recently refined structural model of PdGa and the theoretically predicted PdGa covalent bonding scheme. The hydrogenation experiment has detected no hydrogen uptake in the PdGa, thus preventing in situ hydride formation that leads to a reduction of the catalytic selectivity. We have also determined bulk physical properties (the magnetic susceptibility, the electrical resistivity, the thermoelectric power, the Hall coefficient, the thermal conductivity and the specific heat) of single-crystalline PdGa. The results show that PdGa is a diamagnet with metallic electrical resistivity and moderately high thermal conductivity. The thermoelectric power is negative with complicated temperature dependence, whereas the Hall coefficient is positive and temperature-dependent, indicating complexity of the Fermi surface. Partial fulfillment of the NMR Korringa relation reveals that the charge carriers are weakly correlated. Specific heat measurements show that the density of electronic states (DOS) at the Fermi energy of PdGa is reduced to 15\% of the DOS of the elemental Pd metal.

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