M. Wencka, M. Hahne, A. Kocjan, S. Vrtnik, P. Koželj, D. Korže, Z. Jagličić, M. Sorić, P. Popčević, J. Ivkov, A. Smontara, P. Gille, S. Jurga, P. Tomeš, S. Paschen, A. Ormeci, M. Armbrüster, Yu. Grin, J. Dolinšek
The intermetallic phase InPd is a candidate material for the use as a catalyst in the methanol steam reforming process. To study the connection between the catalytic properties of the surface and the structural and electronic properties of the bulk, we have grown single crystals of the InPd phase by the Czochralski method and determined their electronic, thermal, magnetic and hydrogen-absorption properties. By growing crystals from a high-temperature solution, we could crystallize a slightly off-stoichiometric In-rich composition In1.04Pd0.96, which contained a significant amount of constitutional defects in the lattice (Pd vacancies on the Pd sublattice) to retain the CsCl-type structure. The strongly inhomogeneously broadened 115In NMR spectrum and the high residual (T → 0) electrical resistivity confirmed the presence of constitutional defects. Single crystals of InPd do not absorb hydrogen, as requested for a good hydrogenation catalyst material. Calculated electronic density of states (DOS) shows large contribution of Pd(d) states at the Fermi level. Application of the electron localizability indicator reveals ionic and multi-centre In–Pd interactions stabilizing the crystal structure. The electrical and thermal conductivities of InPd show metallic character, whereas the thermoelectric power and the Hall coefficient both show positive sign, revealing that InPd is a predominant hole-type conductor. The calculated electronic DOS at the Fermi energy is in a good agreement with the experimental value determined from the low-temperature specific heat. Magnetic measurements have shown that InPd is a diamagnet. All results are compared to the chemically related intermetallic compound GaPd. The active–site-isolation concept for increased catalytic selectivity is discussed in relation to the InPd and GaPd structures.