vestichИзвестия Национальной академии наук Беларуси. Серия химических наукProceedings of the National Academy of Sciences of Belarus, Chemical Series1561-83312524-2342The Republican Unitary Enterprise Publishing House "Belaruskaya Navuka"10.29235/1561-8331-2024-60-2-95-104vestich-875Research ArticleФИЗИЧЕСКАЯ ХИМИЯPHYSICAL CHEMISTRYТермическое и химическое расширение слоистых кислороддефицитных двойных перовскитовThermal and chemical expansion of layered oxygen-deficient double perovskitesКлындюкА. И.KlyndyukА. I.

Клындюк Андрей Иванович – кандидат химических наук, доцент

ул. Свердлова, 13а, 220006, Минск

Klyndyuk Andrei I. – Ph. D. (Chemistry), Associate Professor

13a, Sverdlov Str., 220006, Minsk

klyndyuk@belstu.byЖуравлеваЯ. Ю.ZhuravlevaYa. Yu.

Журавлева Яна Юрьевна – аспирант

ул. Свердлова, 13а, 220006, Минск

Zhuravleva Yana Yu. – Postgraduate Student

13a, Sverdlov Str., 220006, Minsk

ya.yu.zhuravleva@mail.ruБелорусский государственный технологический университетBelаrusian State Technological University20242405202460295104Copyright © Клындюк А.И., Журавлева Я.Ю., 20242024Клындюк А.И., Журавлева Я.Ю.Klyndyuk А.I., Zhuravleva Y.Y.Данная работа распространяется под лицензией Creative Commons Attribution 4.0.This work is licensed under a Creative Commons Attribution 4.0 License.https://vestichem.belnauka.by/jour/article/view/875

Слоистые кислороддефицитные двойные перовскиты (КДП) на основе редкоземельных элементов (РЗЭ), бария и 3d-металлов (Fe, Co, Cu и др.) характеризуются высокими электропроводностью и электрохимической активностью в реакции восстановления кислорода, благодаря чему рассматриваются как перспективные катодные материалы для среднетемпературных твердооксидных топливных элементов (ТОТЭ) на основе протон- и кислородионпроводящих твердых электролитов (ТЭ). Эффективные катодные материалы должны быть термомеханически совместимы с материалами ТЭ, что наблюдается в случае близости их коэффициентов термического расширения (КТР). В связи с этим исследование термического расширения КДП, а также выделение различных вкладов в него (термического, химического, спинового и др.) представляет значительный интерес. Дилатометрическим методом исследовано термическое расширение КДП NdBa1–xSrxFeCo0,5Cu0,5O6−δ (0,0 ≤ х ≤ 1,0) (NBSFCC). Установлено, что значения среднего коэффициента линейного термического расширения КЛТР (α) образцов скачкообразно возрастают от (15,1–16,2) · 10–6 К–1 при Т < 630–920 К до (18,9–23,5) · 10–6 К–1 при Т > 630–920 К, что обусловлено выделением из образцов слабосвязанного кислорода. Значения α фаз NBSFCC в низкотемпературном интервале увеличиваются с ростом их индекса кислородной нестехиометрии (δ), а в высокотемпературном – с ростом х, что связано с возрастанием химического вклада в расширение образцов. На основании результатов дилатометрии, термогравиметрии и иодометрии выделены термический и химический вклады в расширение КДП NBSFCC и исследованы их зависимости от типа структуры, катионного и анионного составов фаз NBSFCC. Обнаружено, что значения коэффициента линейного химического расширения (КЛХР, αδ ) образцов сильно возрастают от (8,6–11,8) · 10–3 для х < 0,5 до (12,6–15,8) · 10–3 для х > 0,5 при повышении симметрии твердых растворов NBSFCC. Показано, что установленные в данной работе зависимости КЛТР и КЛХР фаз NBSFCC от их структуры и химического состава хорошо согласуются с аналогичными зависимостями, обнаруженными ранее для других КДП.

Layered oxygen-deficient double perovskites (ODP) based on the rare-earth elements (REE), barium and 3d-metals (Fe, Co, Cu etc.) are characterized by high values of electrical conductivity and high electrochemical activity in oxygen reduction reaction, and are considered as prospective cathode materials for intermediate-temperature solid oxide fuel cells (SOFC) on the base of proton- and oxygen-ion conducting solid electrolytes (SE). Effective cathode materials should be thermomechanically compatible with materials of SE, which tаkes place when the values of their thermal expansion coefficients (TEC) are close to each other. Due to this the study of thermal expansion of ODP as well as the isotation of different contributions in it (thermal, chemical, spin etc.), is of considerable interest. In this work using dilatometric method the thermal expansion of NdBa1–xSrxFeCo0,5Cu0,5O6−δ (0.0 ≤ х ≤ 1.0) (NBSFCC) ODP was studied using dilatometric method. It was established that the values of average linear thermal expansion coefficient (LTEC) (α) of the samples sharply increased from (15.1–16.2) · 10–6 K–1 at Т < 630–920 K to (18.9–23.5) 10–6 K–1 at Т > 630–920 K due to the evolution of weaklybonded oxygen from the samples. Values of α in the low-temperature region increase with increasing of values of their oxygen nonstoichiometry index (δ), and in the high-temperature one increase with the x increasing due to the increment of chemical contribution in the samples expansion. Based of the results of dilatometry, thermogravimetry, and iodometry, the thermal and chemical contributions in the expansion оn NBSFCC were isolated, and the effect of crystal structure, cationic and anionic composition of NBSFCC ODP on the values of their thermal and linear chemical expansion coefficient (LCEC, αδ ) was investigated. It was found, that LCEC values of the samples sharply increased from (8.6–11.8) · 10–3 at (х < 0.5) to (12.6–15.8) · 10–3 at (х > 0.5) when transition from ordered tetragonal (х < 0.5) to disordered cubic (х > 0.5) phase took place. It was shown, that dependences of LTEC and LCEC of NBSFCC phases on their crystal structure and chemical compositions obtained in this work are in good accordance with the analogous dependences determined earlier for the ODP of other types.

слоистые перовскитытвердые растворытермическое расширениехимическое расширениекатодные материалыдилатометриятвердооксидные топливные элементытермогравиметрияиодометрияlayered perovskitessolid solutionsthermal expansionchemical expansioncathode materialsdilatometrysolid oxide fuel cellsthermogravimetryiodometryРентгенографические и термогравиметрические исследования порошков NBSFCC проведены на базе Центра физико-химических методов исследований Белорусского государственного технологического университета (БГТУ). Авторы благодарят кандидата технических наук Н. Н. Гундиловича (кафедра технологии стекла и керамики БГТУ) за запись дилатограмм керамических образцов NBSFCC.X-ray and thermogravimetric studies of NBSFCC powders were carried out at the Center for Physical and Chemical Investigations Methods Center of the Belarusian State Technological University (BSTU). The authors thank Candidate of Technical Sciences N. N. 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The authors declare that there are no conflicts of interest present.