Why do ternary compounds exist? — Thermoanalytical investigations on binary systems of metal chlorides |
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Authors: | H J Seifert |
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Institution: | (1) Inorganic Chemistry, University Gh-Kassel/G.F.R., Germany |
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Abstract: | Ternary chlorides are stable if they can be formed from each pair of the other compounds in a system with a gain in energy. Especially, the energy of formation from the two adjacent compounds, the energy of synproportionation must be negative. At 0 K this condition is fulfilled, if (lattice) enthalpy is won. At higher temperature also theT· S-term of the Gibbs-Helmholtz-equation can be of significance: a loss in H must be compensated by a gain inT· S, if a (high-temperature) compound shall exist.This conception was proved experimentally on systems ACl/MCl2 and ACl/LnCl3(Ln=Lanthanides). By DTA and X-ray powder patterns the phase diagrams of the pseudobinary systems were elucidated, to yield the stoichiometry and structures of the existing compounds. By solution calorimetry the formation enthalpies at room temperature from the binary parent-compounds were determined. Measurements with a galvanic cell for solid electrolytes at temperatures higher than 300 °C yield the free enthalpies and entropies of synproportionation.The main result of these measurements is, that compounds with isolated coordination polyhedra (K2CoCl4=tetrahedra; Rb3LaCl6=octahedra) can have a sufficiently high gain in entropy to be stable at temperatures > 0 K.
Zusammenfassung Ternäre Chloride sind stabil, wenn sie sich aus allen Paaren der restlichen in einem System existierenden Verbindungen unter Energiegewinn darstellen lassen. Insbesondere muß die Bildungsenergie aus den beiden Nachbarverbindungen, die Synproportionierungsenergie, netativ sein. Bei 0 K ist diese Bedingung erfüllt, wenn dabei (Gitter-) Enthalpie gewonnen wird. Bei höheren Temperaturen kann auch derT· S-Term der Gibbs-Helmholtz-Gleichung ausschlaggebend werden: ein Verlust an H muß durch einen genügend großen Gewinn anT· S kompensiert werden, damit eine (Hochtemperatur-) Verbindung existieren kann.Dieses Konzept wurde experimentell an Systemen ACl/MCl2 und ACl/LnCl3 (Ln=Lanthanoid) bewiesen. Durch DTA und Röntgenpulveraufnahmen wurden die Phasendiagramme der pseudobinären Systeme erstellt, um Zusammensetzung und Strukturen der existierenden Verbindungen zu ermitteln. Mittels Lösungskalorimetrie wurden die Bildungsenthalpien bei Raumtemperaturen aus den binären Ausgangsverbindungen gemessen. Messungen mit einer galvanischen Zelle für Festelektrolyte bei Temperaturen >300 °C lieferten die freien Enthalpien und Entropien für die Synproportionierungsreak-tionen. Als wichtigstes Resultat ergab sich, daß Verbindungen mit isolierten Koordinationspolyedern (K2CoCl4=Tetraeder; Rb3LaCl6=Oktaeder) einen so großen Entropiegewinn aufweisen, daß sie bei hohen Temperaturen stabil sein können.
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![icy](/content/xm414786050q22n0/xxlarge1080.gif) ![ecy](/content/xm414786050q22n0/xxlarge1101.gif) ![dcy](/content/xm414786050q22n0/xxlarge1076.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ( 2![Scy](/content/xm414786050q22n0/xxlarge1057.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) l4 — ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![iecy](/content/xm414786050q22n0/xxlarge1077.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![ecy](/content/xm414786050q22n0/xxlarge1101.gif) ![dcy](/content/xm414786050q22n0/xxlarge1076.gif) , RbLaCl6 — ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![kcy](/content/xm414786050q22n0/xxlarge1082.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![ecy](/content/xm414786050q22n0/xxlarge1101.gif) ![dcy](/content/xm414786050q22n0/xxlarge1076.gif) ) ![mcy](/content/xm414786050q22n0/xxlarge1084.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![gcy](/content/xm414786050q22n0/xxlarge1075.gif) ![ucy](/content/xm414786050q22n0/xxlarge1091.gif) ![icy](/content/xm414786050q22n0/xxlarge1080.gif) ![mcy](/content/xm414786050q22n0/xxlarge1084.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![dcy](/content/xm414786050q22n0/xxlarge1076.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![scy](/content/xm414786050q22n0/xxlarge1089.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![chcy](/content/xm414786050q22n0/xxlarge1095.gif) ![ncy](/content/xm414786050q22n0/xxlarge1085.gif) ![ycy](/content/xm414786050q22n0/xxlarge1099.gif) ![icy](/content/xm414786050q22n0/xxlarge1080.gif) ![zcy](/content/xm414786050q22n0/xxlarge1079.gif) ![bcy](/content/xm414786050q22n0/xxlarge1073.gif) ![ycy](/content/xm414786050q22n0/xxlarge1099.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![ecy](/content/xm414786050q22n0/xxlarge1101.gif) ![ncy](/content/xm414786050q22n0/xxlarge1085.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![pcy](/content/xm414786050q22n0/xxlarge1087.gif) ![icy](/content/xm414786050q22n0/xxlarge1080.gif) , ![chcy](/content/xm414786050q22n0/xxlarge1095.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![ocy](/content/xm414786050q22n0/xxlarge1086.gif) ![bcy](/content/xm414786050q22n0/xxlarge1073.gif) ![bcy](/content/xm414786050q22n0/xxlarge1073.gif) ![ycy](/content/xm414786050q22n0/xxlarge1099.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![bcy](/content/xm414786050q22n0/xxlarge1073.gif) ![icy](/content/xm414786050q22n0/xxlarge1080.gif) ![lcy](/content/xm414786050q22n0/xxlarge1083.gif) ![softcy](/content/xm414786050q22n0/xxlarge1100.gif) ![ncy](/content/xm414786050q22n0/xxlarge1085.gif) ![ycy](/content/xm414786050q22n0/xxlarge1099.gif) ![mcy](/content/xm414786050q22n0/xxlarge1084.gif) ![pcy](/content/xm414786050q22n0/xxlarge1087.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![iecy](/content/xm414786050q22n0/xxlarge1077.gif) ![mcy](/content/xm414786050q22n0/xxlarge1084.gif) ![pcy](/content/xm414786050q22n0/xxlarge1087.gif) ![iecy](/content/xm414786050q22n0/xxlarge1077.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![tcy](/content/xm414786050q22n0/xxlarge1090.gif) ![ucy](/content/xm414786050q22n0/xxlarge1091.gif) ![rcy](/content/xm414786050q22n0/xxlarge1088.gif) ![acy](/content/xm414786050q22n0/xxlarge1072.gif) ![vcy](/content/xm414786050q22n0/xxlarge1074.gif) ![ycy](/content/xm414786050q22n0/xxlarge1099.gif) ![shcy](/content/xm414786050q22n0/xxlarge1096.gif) .
Support by the Deutsche Forschungsgemeinschaft and Fonds der Chemischen Industry is gratefully acknowledged. |
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