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ZrO2–ZnO–CeO2 integrated with nano-sized SAPO-34 zeolite for CO2 hydrogenation to light olefins

Granule oxides of ZrO 2 –ZnO–CeO 2 are integrated with nano - sized SAPO-34 zeolites to form tandem catalyst, which is effectively utilized in catalysis of CO 2 hydrogenation to produce light olefins. Then, Nano-sized SAPO-34 zeolite of particle diameter about 100 nm is synthesized by using morpholi...

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Published in:Reaction kinetics, mechanisms and catalysis mechanisms and catalysis, 2022-12, Vol.135 (6), p.2959-2972
Main Authors: Nan, Yongyong, Mao, Yuzhong, Zha, Fei, Yang, Zirong, Ma, Shizi, Tian, Haifen
Format: Article
Language:English
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Summary:Granule oxides of ZrO 2 –ZnO–CeO 2 are integrated with nano - sized SAPO-34 zeolites to form tandem catalyst, which is effectively utilized in catalysis of CO 2 hydrogenation to produce light olefins. Then, Nano-sized SAPO-34 zeolite of particle diameter about 100 nm is synthesized by using morpholine-treated SAPO-34 as seed of crystal and taking morpholine as the sole template. Ternary ZrO 2 –ZnO–CeO 2 oxides with various CeO 2 contents are prepared by traditional co-precipitation method. The catalysts were characterized by XRD, SEM, TEM, N 2 adsorption–desorption, H 2 -TPR, NH 3 -TPD, CO 2 -TPD, XPS and in situ DRIFT measurements. The introduction of CeO 2 into Zr-Zn oxides efficiently increases the oxygen vacancies to possess the stronger adsorption capacity of CO 2 and H 2 . Nano-sized SAPO-34 has a larger specific surface area and suitable amount of medium to strong acidic sites. CO 2 conversion and products distribution are strongly dependent on the oxide composition and morphology of SAPO-34 zeolite. When the atomic ratio of Zr:Zn:Ce is 4:2:1, the mass ratio of metal oxide to zeolite is 1:1, under the reaction temperature of 350 °C, pressure of 2.6 MPa, CO 2 :H 2  = 1:3 (molar ratio), GHSV = 6000 mL/(g cat h) and the tandem catalyst dosage of 0.5 g, the CO 2 conversion is 24.1%, the selectivity and yield of light olefins are 86.3% and 20.8%, respectively, and the catalytic lifetime is about 425 min.
ISSN:1878-5190
1878-5204
DOI:10.1007/s11144-022-02319-2