Подвижность кислорода допированных самарием никелатов неодима, спеченных электронными пучками

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Фазы Раддлесдена–Поппера являются известными материалами электрохимических устройств, таких как твердооксидные топливные элементы/электролизеры, кислородпроводящие мембраны. Допирование A-положения лантаноидами меньшего радиуса может помочь увеличить кислородную подвижность, однако данный вопрос до сих пор мало исследован. Настоящая работа посвящена изучению фазового состава и транспортных свойств допированных Sm никелатов Nd, спеченных радиационно-термическим методом с использованием электронных пучков. Nd2–xSmxNiO4+δ (x = 0.2, 0.4) были синтезированы модифицированным методом Пекини и спечены электронными пучками при 1150–1250°C. Полученные материалы охарактеризованы с помощью рентгенофазового анализа, рентгеновской фотоэлектронной спектроскопии и термопрограммированного изотопного обмена с C18O2 в проточном реакторе. Кислород поверхности материалов представлен в виде двух форм с различной энергией связи. По данным термопрограммированного изотопного обмена кислорода, для образцов характерна неоднородность подвижности кислорода, причем при x = 0.4 образуется канал медленной диффузии. Данные особенности диффузии кислорода, по-видимому, связаны с влиянием допирования и радиационно-термического спекания на структуру с образованием примесных фаз, нарушением кооперативного механизма диффузии за счет локальных дефектов и изменения состава поверхности и междоменных границ.

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В. А. Садыков

Институт катализа им. Г.К. Борескова СО РАН

Автор, ответственный за переписку.
Email: sadykov@catalysis.ru
Россия, Новосибирск

Е. М. Садовская

Институт катализа им. Г.К. Борескова СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

Ю. Н. Беспалко

Институт катализа им. Г.К. Борескова СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

Е. А. Смаль

Институт катализа им. Г.К. Борескова СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

О. А. Булавченко

Институт катализа им. Г.К. Борескова СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

Н. Ф. Еремеев

Институт катализа им. Г.К. Борескова СО РАН

Email: yeremeev21@catalysis.ru
Россия, Новосибирск

И. П. Просвирин

Институт катализа им. Г.К. Борескова СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

М. А. Михайленко

Институт химии твердого тела и механохимии СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

М. В. Коробейников

Институт ядерной физики им. Г.И. Будкера СО РАН

Email: sadykov@catalysis.ru
Россия, Новосибирск

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2. Рис. 1. Дифрактограммы образцов Nd1.8Sm0.2NiO4+δ, спеченных РТС при 1150°C (1) и 1250°C (2). Обозначение фаз: * – (Nd, Sm)2NiO4+δ (ICSD50440), ^ – (Nd, Sm)2O3 (ICSD60639), ↓ – NiO.

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3. Рис. 2. Дифрактограммы образцов Nd1.6Sm0.4NiO4+δ, спеченных РТС при 1150°C (1) и 1250°C (2). Обозначение фаз: * – (Nd, Sm)2NiO4+δ (ICSD50440), ♦ – (Nd, Sm)NiO3-δ (PDF 00–041–0344).

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4. Рис. 3. O1s РФЭС спектры образцов Nd1.8Sm0.2NiO4+δ, спеченных в печи при 1150°C (1), РТС при 1150°C (2), образца Nd1.6Sm0.4NiO4+δ, спеченного РТС при 1150°C (3), и образца Nd1.8Sm0.2NiO4+δ, спеченного РТС при 1250°C (4).

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5. Рис. 4. Термопрограммированный изотопный обмен кислорода с C18O2 в проточном реакторе для образцов Nd2–xSmxNiO4+δ (x = 0.2 и 0.4), спеченных РТС при различных температурах. Точки – эксперимент, линии – модель.

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6. Рис. 5. Зависимость коэффициента самодиффузии кислорода для образцов Nd2-xSmxNiO4+δ, спеченных в печи и РТС, по данным ТПИО C18O2: (1) Nd2NiO4+δ, спеченного в печи при 1150°C [36], (2) Nd1.8Sm0.2NiO4+δ, спеченного в печи при 1150°C [35], (3) Nd1.8Sm0.2NiO4+δ, спеченного РТС при 1150°C (данная работа), (4) Nd1.8Sm0.2NiO4+δ, спеченного РТС при 1250°C (данная работа), (5, 5ʹ) Nd1.6Sm0.4NiO4+δ, спеченного РТС при 1150°C (данная работа).

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