Abstract
AbstractNeedle‐shaped crystals of Eu5Zr3S12 and Eu3.67Sr1.33Zr3S12 were synthesized by solid‐state reactions of the elements and ZrS2 at 673–1273 K in alumina crucibles, and their crystal structures were determined by single‐crystal methods. They are isotypic with hexagonal symmetry (space group P2m, Z = 1, Eu5Zr3S12: a = 1170.7(2), c = 394.27(8) pm, wR2 = 0.0636 for 552 F2 and 27 parameters; Eu3.67Sr1.33Zr3S12: a = 1167.0(2), c = 395.71(8) pm, wR2 = 0.0887 for 484 F2 and 29 parameters) and contain one‐dimensional chains of edge‐sharing ZrS2S4/2 octahedra running parallel to [001]. Two europium sites are seven‐ or ninefold‐coordinated by sulfur. Eu5Zr3S12 is a Curie paramagnet with an effective magnetic moment of μeff = 13.37(1) μB per formula unit (fu), in agreement with three Eu2+/fu. 151Eu Mössbauer spectra show two absorption lines suggesting a static mixture of Eu2+ and Eu3+ in accordance with Eu32+Eu23+Zr34+S122–.This assignment is not in line with the observed Eu–S distances. To resolve this, we suggest pure Eu2+ at the 2c site and inhomogeneous mixed valence at the 3f site according to (Eu22+)2c(Eu2+Eu23+)3fZr34+S122–. This is supported by the site preference of Sr2+ in Eu3.67Sr1.33Zr3S12.
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