Термодинамическая устойчивость и физико-химические свойства двойных перовскитов YBaCo2O6-δ и HoBaCo2O6-δ : диссертация на соискание ученой степени кандидата химических наук : 02.00.04

Введение …………………………………………………………………………………………………………………………. 4
1 Литературный обзор ……………………………………………………………………………………………………………… 10
1.1 Кристаллическая структура сложных оксидов RBaCo2O6-δ (где R – редкоземельный
элемент) ……………………………………………………………………………………………………………………….. 10
1.1.1 Влияние кислородной нестехиометрии на кристаллическую решетку RBaCo 2O6-δ ……………….. 11
1.1.2 Влияние радиуса редкоземельного иона R3+ на кристаллическую структуру RBaCo2O6-δ………. 16
1.1.3 Влияние температуры на кристаллическую структуру RBaCo2O6-δ ……………………………………….. 19
1.2 Термодинамическая устойчивость RBaCo2O6-δ………………………………………………………………………. 20
1.3 Зависимость содержания кислорода RBaCo2O6-δ от температуры ………………………………………….. 26
1.3.1 Кислородная нестехиометрия YBaCo2O6-δ и HoBaCo2O6-δ …………………………………………………….. 27
1.4 Электропроводность двойных перовскитов RBaCo2O6-δ ………………………………………………………… 30
1.5 Дефектная структура двойных перовскитов RBaCo2O6-δ…………………………………………………………. 33
1.6 Термодинамика двойных перовскитов ………………………………………………………………………………… 36
2 Постановка задачи исследования …………………………………………………………………………………………… 38
3 Методика эксперимента ………………………………………………………………………………………………………… 40
3.1 Синтез образцов …………………………………………………………………………………………………………………. 40
3.2 Метод рентгенофазового анализа ……………………………………………………………………………………….. 41
3.3 Изготовление керамических образцов ………………………………………………………………………………… 42
3.4 Измерение общей электропроводности ………………………………………………………………………………. 42
3.5 Кулонометрическое титрование ………………………………………………………………………………………….. 44
3.6 Термогравиметрический анализ ………………………………………………………………………………………….. 48
3.7 Методика определения абсолютной нестехиометрии прямым восстановлением образца в токе
водорода ……………………………………………………………………………………………………………………….. 49
3.8 Определение абсолютной кислородной нестехиометрии окислительно-восстановительным
титрованием ……………………………………………………………………………………………………………………….. 49
3.9 Метод гомогенизирующих отжигов …………………………………………………………………………………….. 51
3.10 Калориметрия сброса………………………………………………………………………………………………………… 52
4 Результаты и их обсуждение ………………………………………………………………………………………………….. 54
4.1 Особенности синтеза двойного перовскита YBaCo2O6-δ …………………………………………………………. 54
4.2 Аттестация синтезированных YBaCo2O6-δ и HoBaCo2O6-δ …………………………………………………………. 61
4.3 Термодинамическая устойчивость YBaCo2O6-δ ………………………………………………………………………. 63
4.4 Термодинамическая устойчивость HoBaCo2O6-δ ……………………………………………………………………. 69
4.5 Содержание кислорода в RBaCo2O6-δ (R = Y, Ho) на воздухе …………………………………………………… 76
4.6 Анализ дефектной структуры RBaCo2O6-δ (R = Y, Ho) ………………………………………………………………. 77
4.7 Парциальная мольная энтальпия кислорода для YBaCo2O6-δ и HoBaCo2O6-δ ……………………………. 84
4.8 Общая электропроводность YBaCo2O6-δ и HoBaCo2O6-δ…………………………………………………………… 88
4.9 Энтальпия окисления и инкременты энтальпии YBaCo2O6-δ …………………………………………………… 91
Заключение ……………………………………………………………………………………………………………………….. 97
Список сокращений и условных обозначений………………………………………………………………………….. 101
Список использованных источников ……………………………………………………………………………………….. 103

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