Editors: | F. Kongoli, M. Haumann, P. Wasserscheid, T. Welton, M. Gaune-Escard, A. Angell, A. Riisager |
Publisher: | Flogen Star OUTREACH |
Publication Year: | 2018 |
Pages: | 154 pages |
ISBN: | 978-1-987820-86-7 |
ISSN: | 2291-1227 (Metals and Materials Processing in a Clean Environment Series) |
Dissolution reactions of transition metal oxides (e.g. V<sub>2</sub>O<sub>5</sub>, Nb<sub>2</sub>O<sub>5</sub>, MoO<sub>3</sub>, WO<sub>3</sub>) in molten pyrosulfate, and formation of the corresponding molten metal oxosulfato complexes [1-4] have expanded our knowledge on coordination chemistry of the pertinent transition metals, and provided a very useful family of coordination complexes as reference compounds for understanding the molecular structure of supported metal oxides, commonly used as catalysts [5]. Herein, we show that the oxide of a heptavalent transition metal, Re<sub>2</sub>O<sub>7</sub> (m.p. 297°C), undergoes likewise a reaction-induced dissolution in molten potassium pyrosulfate. Large amounts of Re<sub>2</sub>O<sub>7</sub> can be dissolved in molten K<sub>2</sub>S<sub>2</sub>O<sub>7</sub> (i.e. a mixture with X(Re<sub>2</sub>O<sub>7</sub>) = 0.5 fuses readily at 260°C). The structural and vibrational properties of molten Re(VII)I oxosulfato complexes formed in binary Re<sub>2</sub>O<sub>7</sub>-K<sub>2</sub>S<sub>2</sub>O<sub>7</sub> (as well as ternary Re<sub>2</sub>O<sub>7</sub>-K<sub>2</sub>S<sub>2</sub>O<sub>7</sub>-K<sub>2</sub>SO<sub>4</sub>) molten mixtures under O<sub>2</sub> atmosphere and static equilibrium conditions are studied by Raman spectroscopy at temperatures of 260-470°C. The corresponding composition effects are explored in the X(Re<sub>2</sub>O<sub>7</sub>) = 0 - 1 range. A quantitative exploitation of the relative Raman band intensities, due to the species present at static equilibrium, allows to determine the stoichiometry of the reaction taking place in the binary system [Re<sub>2</sub>O<sub>7</sub> + nS<sub>2</sub>O<sub>7</sub>(2-) = C(2n-)] pointing to n = 1. Temperature and composition dependent evolutions of molecular structures and configurations are discussed and consistent band assignments are proposed.