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Crystal Structures of the High‐Pressure Palladium Dichalcogenides Pd 0.94(1) S 2 and Pd 0.88(1) Se 2 Comprising Exceptional Pd IV Oxidation States
Author(s) -
Selb Elisabeth,
Götsch Thomas,
Janka Oliver,
Penner Simon,
Heymann Gunter
Publication year - 2017
Publication title -
zeitschrift für anorganische und allgemeine chemie
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.354
H-Index - 66
eISSN - 1521-3749
pISSN - 0044-2313
DOI - 10.1002/zaac.201700140
Subject(s) - palladium , crystallography , crystal structure , chemistry , x ray photoelectron spectroscopy , high pressure , orthorhombic crystal system , metastability , diamagnetism , analytical chemistry (journal) , materials science , catalysis , nuclear magnetic resonance , thermodynamics , physics , biochemistry , organic chemistry , quantum mechanics , chromatography , magnetic field
Metastable palladium deficient high‐pressure phases with the compositions Pd 1– x S 2 and Pd 1– x Se 2 could be obtained via high‐pressure/high‐temperature syntheses at 7.5 GPa (Pd 0.88(1) Se 2 ) and 11.5 GPa (Pd 0.94(1) S 2 ) at 1523 K. Compared to the normal‐pressure modifications they showed a significant decrease in the c ‐lattice parameters of Δ c/c = 4.4 % (Pd 0.94(1) S 2 ) and Δ c/c = 10.8 % (Pd 0.88(1) Se 2 ) accompanied by under‐occupied palladium sites. Single‐crystal analyses indicated the space group Pbca with lattice parameters and refinement results of a = 552.02(8), b = 555.11(8), c = 720.20(11) pm, R 1 = 0.0562, wR 2 = 0.0710 (all data) for Pd 0.94(1) S 2 and a = 587.93(3), b = 593.16(4), c = 685.99(4) pm, R 1 = 0.0139, wR 2 = 0.0232 (all data) for Pd 0.88(1) Se 2 . XPS investigations revealed a partial oxidation of Pd 2+ to Pd 4+ , which was observed for the first time in palladium chalcogenide chemistry. Magnetic susceptibility measurements confirmed the expected diamagnetic behavior.

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