catalКатализ в промышленностиKataliz v promyshlennosti1816-03872413-6476LLC "KALVIS"10.18412/1816-0387-2024-6-35-47catal-1082Research ArticleКАТАЛИЗ В ХИМИЧЕСКОЙ И НЕФТЕХИМИЧЕСКОЙ ПРОМЫШЛЕННОСТИCATALYSIS IN CHEMICAL AND PETROCHEMICAL INDUSTRYРазработка новых каталитических материалов для водородной энергетики на основе Ni-Co наносплавов на поверхности наноструктурированной (Ni)CoAl2O4 шпинели и их исследование в реакции углекислотной конверсии метанаThe surface of nanostructured (Ni)CoAl2O4 spinel and their study in dry reforming of methaneШутиловА. А.ShutilovA. A.ctls@kalvis.ruСимоновМ. Н.SimonovM. N.ctls@kalvis.ruФедороваВ. Е.FedorovaV. E.ctls@kalvis.ruМарчукА. С.MarchukA. S.ctls@kalvis.ruПросвиринИ. П.ProsvirinI. P.ctls@kalvis.ruСадовскаяЕ. М.SadovskayaE. M.ctls@kalvis.ruЕремеевН. Ф.EremeevN. F.ctls@kalvis.ruЗенковецГ. А.ZenkovetsG. A.ctls@kalvis.ruИнститут катализа СО РАН, НовосибирскРоссияBoreskov Institute of catalysis, NovosibirskRussian Federation2024101220242463547Copyright © LLC "KALVIS", 20242024LLC "KALVIS"LLC "KALVIS"https://www.catalysis-kalvis.ru/jour/about/submissions#copyrightNoticehttps://www.catalysis-kalvis.ru/jour/article/view/1082

Катализаторы состава NixCo1–xAl2O4 (x = 0÷0,5) готовили методом соосаждения растворов азотнокислых солей Ni, Co и Al. При термообработке полученного ксерогеля при 700 °С на воздухе формируется оксид алюминия со структурой шпинели, в котором стабилизированы ионы никеля и кобальта. Изучение in situ восстановления этих прекурсоров в водородсодержащей газовой смеси при 700 °С методом рентгенофазового анализа и ex situ после предварительного восстановления в водородсодержащей газовой смеси и дальнейшей работы в условиях реакционной среды показало, что на поверхности шпинели формируются ансамбли частиц сплава Ni-Co размером 3-4 нм. Исследовано влияние состава катализаторов и продолжительности их испытания на каталитические свойства в реакции углекислотной конверсии метана (УКМ). Катализатор состава Ni0,35Co0,65Al2O4 показал стабильную работу в реакции УКМ в течение 20 ч при конверсии CH4 76 % и выходе H2 42 % (Т = 700 °C, τ = 30 мс). Высокая каталитическая активность полученных катализаторов в УКМ обусловлена формированием высокодисперсных сплавных Ni-Co наночастиц активной фазы в количестве 17–18 мас.% на изначально большой удельной поверхности шпинели, стабилизированной ионами никеля и кобальта, и обладающей подвижным объемным кислородом в восстановленном состоянии.

NixCo1-xAl2O4 (x = 0–0.5) catalysts were prepared by the co-precipitation from solution of Ni, Co and Al nitrates. The dry gel was heated at 700 °C in air and resulting alumina modified by nickel and cobalt ions is formed with spinel structure. The in situ X-ray diffraction study of these precursors in the reduction by a H2-containing gas mixture at 700 °C and ex situ after preliminary reduction in a H2-containing gas mixture and further work under reaction medium conditions  showed that ensembles of Ni-Co alloy particles 3-4 nm in size are formed on the spinel surface. The influence of the composition of the catalysts and the duration of their testing on the catalytic properties in the dry reforming of methane reaction (DRM) was studied. The Ni0.35Co0.65Al2O4 catalyst is stable in the DRM for 20 hours with CH4 conversion of 76 % and an H2 yield of 42 % (T = 700 °C, t = 30 ms). The high catalytic activity of the obtained catalysts in DRM is due to the formation of highly dispersed (3–4 nm) nanoparticles of the Ni-Co alloy an active phase in an amount of 17–18 wt. % on the initially large specific surface area of a spinel, stabilized by nickel and cobalt ions, and possessing mobile bulk oxygen under reducing reaction conditions.

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