alternativeАльтернативная энергетика и экология (ISJAEE)Alternative Energy and Ecology (ISJAEE)1608-8298Международный издательский дом научной периодики "Спейс10.15518/isjaee.2017.25-27.013-023alternative-1159Research ArticleСтатьиПРИГОТОВЛЕНИЕ И ИССЛЕДОВАНИЕ КЕРАМИЧЕСКОГО МЕМБРАННОГО РЕАКТОРА ДЛЯ КАТАЛИТИЧЕСКОГО РАЗЛОЖЕНИЯ СЕРОВОДОРОДАPREPARATION AND STUDY OF CERAMIC MEMBRANE REACTOR FOR HYDROGEN SULFIDE CATALYTIC DECOMPOSITIONХайрулинС. Р.KhairulinS. R.

канд. хим. наук, заведующий лабораторией экологического катализа

Ph.D. (chemistry), Head of Laboratory of Environmental Catalysis

sergk@catalysis.ruКузнецовВ. В.KuznetsovV. V.

инженер

Engineer D.Sc. (chemistry), Senior Researcher

sergk@catalysis.ruПодъячеваО. Ю.PodyachevaO. Yu.

д-р хим. наук, старший научный сотрудник

D.Sc. (chemistry), Senior Researcher

sergk@catalysis.ruИсмагиловЗ. Р.IsmagilovZ. R.

д-р хим. наук, профессор, чл.-корр. РАН, директор Института углехимии и химического материаловедения Федерального исследовательского центра угля и углехимии CО РАН

D.Sc. (chemistry), Professor, Corresponding Member of RAS, Director of Institute of Coal Chemistry and Material Science of Federal Research Centre of Coal and Coal Chemistry SB RAS

zinfer1@mail.ruИнститут катализа им. Г. К. Борескова СО РАНРоссияBoreskov Institute of Catalysis SB RASRussian FederationИнститут катализа им. Г. К. Борескова СО РАН; Институт углехимии и химического материаловедения СО РАНРоссияBoreskov Institute of Catalysis SB RAS; Institute of Coal Chemistry and Material Science SB RASRussian Federation201709122017025-271323Copyright © Международный издательский дом научной периодики "Спейс, 20172017Международный издательский дом научной периодики "СпейсМеждународный издательский дом научной периодики "Спейсhttps://www.isjaee.com/jour/about/submissions#copyrightNoticehttps://www.isjaee.com/jour/article/view/1159

В статье исследовалась серия керамических мембранных катализаторов на основе оксида алюминия различного состава для реакции высокотемпературного разложения сероводорода. Использовались два типа каталитических мембран слоистой структуры: первый тип включал слой катализатора, носитель мембраны и мембранный слой, а второй – слой катализатора, носитель мембраны, промежуточный слой и мембранный слой. В статье приведены физико-химические характеристики (пористая структура, удельная поверхность, фазовый состав) носителя мембраны и мембранного слоя, прокаленных при различной температуре. Детально описана методика приготовления мембранных реакторов различной структуры. Приведены данные по исследованию проницаемости мембранных реакторов по H2 и H2S. Описаны результаты испытаний приготовленных мембран в реакции разложения H2S в диапазоне температур 600–900 ºС. Показано, что введение добавок La2O3 в состав мембранного слоя приводит к увеличению термической стабильности мембраны. Эффективный диаметр пор мембранного слоя состава 5%La2O3-γ-Al2O3, прокаленного при 900 ºС, был в три раза меньше, чем немодифицированного γ-Al2O3. Кроме того, в составе модифицированного мембранного слоя наблюдалось только присутствие фазы γ-Al2O3, а в немодифицированном образце наблюдалось образование фазы δ-Al2O3. Показано, что пористая структура и толщина мембранного слоя значительно влияют на проницаемость H2 и H2S. В результате того, что отношение коэффициентов проницаемости H2/H2S больше 2,5, наблюдалось значительное улучшение каталитической активности в реакции разложения H2S по сравнению с гранулированным катализатором. Введение в состав мембраны промежуточного слоя, отличающегося от мембранного слоя эффективным диаметром пор, привело к существенному увеличению степени превращения H2S. Показано, что мембранный реактор, содержащий в своем составе мембранный слой толщиной 6 мкм с эффективным диаметром пор 45 Å и промежуточный слой толщиной 9 мкм с диаметром пор 110 Å, демонстрировал максимальную эффективность в реакции разложения сероводорода. Степень превращения H2S достигала 70 % при 900 ºС на мембранном катализаторе оптимального состава.

 

The paper studies a number of alumina ceramic membrane catalysts of various design and composition for high temperature H2S decomposition. The design of two types of catalytic membranes used consists of sandwich-like structure including (1) “catalytic layer”/”membrane support”/”membrane layer” and (2) “catalytic layer”/”membrane support”/”intermediate layer”/”membrane layer”. The paper describes: the physical and chemical properties (pore structure, specific surface area and phase composition) of membrane supports and membrane layers calcined at different temperatures; the methods of various composition membrane reactors preparation; the data on membrane permeability on H2 and H2S; the test results of prepared membranes in the reaction of H2S decomposition. The introduction of La2O3 modifying additions in a membrane layer is shown to lead to the increase of thermal stability of a membrane. The effective diameter of pores of membrane layer having 5%La2O3-γ-Al2O3 composition and calcined at 900ºC is three times lower than of the unmodified γ-Al2O3. The presence of pure γ-Al2O3 phase in the modified membrane layer is observed while the δ-Al2O3 phase is formed in the unmodified sample. The pore structure and the thickness of the membrane layer are demonstrated to significantly influence permeability of H2 and H2S. There has been observed a significant improvement of the catalytic activity in the H2S decomposition reaction compared with a granulated catalyst because the separation coefficient of H2/H2S is higher than 2.5. It has been determined that the introduction an intermediate layer, which has different effective pore diameter in comparison with the membrane layer, to the membrane composition increases significantly the H2S conversion. The membrane reactor consisting of the membrane layer (6 m thickness, pore diameter 45 Å) and the intermediate layer (9 m thickness, pore diameter 110 Å) has been found to exhibit maximal efficiency in the H2S decomposition reaction. The H2S conversion reaches 65% at 900ºC on the membrane catalyst of optimal composition.

 

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The authors declare that there are no conflicts of interest present.