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The Role of Protons and Formation Cu(NH3)2+ During Ammonia-Assisted Solid-State Ion Exchange of Copper(I) Oxide into Zeolites Научная публикация

Журнал Topics in Catalysis
ISSN: 1022-5528 , E-ISSN: 1572-9028
Вых. Данные Год: 2019, Том: 62, Номер: 1-4, Страницы: 100-107 Страниц : 8 DOI: 10.1007/s11244-018-1096-x
Авторы Vennestrøm Peter N.R. 1 , Lundegaard Lars F. 2 , Tyrsted Christoffer 2 , Bokarev Dmitriy A. 3 , Mytareva Alina I. 3 , Baeva Galina N. 3 , Stakheev Alexandr Y. 3 , Janssens Ton V.W. 1
Организации
1 Umicore Denmark ApS, Kgs. Lyngby, Denmark
2 Haldor Topsoe A/S, Kgs. Lyngby, Denmark
3 N.D. Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, Moscow, Russia

Реферат: Solid-state ion exchange in mixtures of copper oxides and zeolites can occur at temperatures as low as 200–250 °C in the presence of ammonia (NH3-SSIE), thus providing a low-temperature method to activate zeolites for selective catalytic reduction nitrogen oxide (NH3-SCR). The ammonia induced solid-state ion exchange process is studied in more detail, by monitoring the development of NH3-SCR activity with duration of NH3-SSIE, formation of a mobile linear [Cu(NH3)2]+ complex with X-ray spectroscopy, and the transfer of Cu to the zeolite by XRD, and evaporation of copper(I)-oxide by TGA. We find that the linear [Cu(NH3)2]+ complex is formed in mixtures of copper-oxide and *BEA and CHA zeolites upon exposure to ammonia. Increasing the temperature for NH3-SSIE to well above 300 °C leads to a less efficient Cu-transfer. This indicates that the [Cu(NH3)2]+ complex is crucial for the NH3-SSIE process. The non-monotonous development of NOx conversion and N2O yield with duration of NH3-SSIE is probably due to an initial enrichment of Cu in the outer shell of the zeolite crystals. We also show that the presence of H+ or NH4+-ions in the zeolite are necessary for the NH3-SSIE, and that the transfer of Cu from the Cu-oxides to the zeolites most likely occurs via a surface diffusion process.
Библиографическая ссылка: Vennestrøm P.N.R. , Lundegaard L.F. , Tyrsted C. , Bokarev D.A. , Mytareva A.I. , Baeva G.N. , Stakheev A.Y. , Janssens T.V.W.
The Role of Protons and Formation Cu(NH3)2+ During Ammonia-Assisted Solid-State Ion Exchange of Copper(I) Oxide into Zeolites
Topics in Catalysis. 2019. V.62. N1-4. P.100-107. DOI: 10.1007/s11244-018-1096-x WOS Scopus OpenAlex
Идентификаторы БД:
≡ Web of science: WOS:000461821000014
≡ Scopus: 2-s2.0-85057777301
≡ OpenAlex: W2903016932
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