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Metal oxide catalysts for the CO₂-assisted propane oxidative dehydrogenation
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Wang, Hedun. Metal oxide catalysts for the CO₂-assisted propane oxidative dehydrogenation. Retrieved from https://doi.org/doi:10.7282/t3-r3ek-sz29

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TitleMetal oxide catalysts for the CO₂-assisted propane oxidative dehydrogenation
NameWang, Hedun (author); Tsilomelekis, George (chair); Celik, Fuat (member); Asefa, Teddy (member); Shapley, Nina (member); Rangarajan, Srinivas (member); Rutgers University; School of Graduate Studies
Date Created2022
Other Date2022-01 (degree)
SubjectChemical engineering, Catalyst stability and deactivation, CO₂ activation, Fe-doped cerium oxide, Mars-van-Krevelen kinetic model, Propane oxidative dehydrogenation
Extent184 pages : illustrations
DescriptionPropylene is one of the most crucial building blocks in chemical and petrochemical industry. In the big picture of shale gas revolution and global warming, the CO₂-assissted propane oxidative dehydrogenation exhibits its unique advantages and stands out as a ‘on-purpose’ propylene production technique. In this work, we endeavor to present a catalyst design idea for both propane and CO₂ activation with high efficiency. Cerium oxide has been well-established with superb oxygen mobility and abundant surface oxygen vacancies, which can be further improved with a transition metal dopant such as Fe, thus giving it great potential to serve as active sites and to maintain long-lasting constant performances. Furthermore, we investigated and evaluated the possibility of anchoring CrOₓ on top of Fe-doped cerium oxide surface and discussed the structure-reactivity relationship of Cr/Fe-CeO₂ catalysts.

Catalytic performances and kinetics of CO₂-assissted propane oxidative dehydrogenation was studied over Fe-doped ceria supported Cr oxides. The catalysts were synthesized via co-precipitation of Fe, Ce, and wetness impregnation of Cr. A pseudo-binary phase Cr/Fe-CeO₂ structure was confirmed after combining Raman, XRD and TEM analysis. H₂-TPR experiments confirmed that the addition of Cr oxides altered original surface oxygen sites and enhanced the reducibility of the catalyst. The Cr-related catalysts outperformed Fe-doped ceria at low reaction temperature range, but as temperature increases the propane dry reforming plays a dominate role and diminished differences in catalytic performance of Fe-CeO₂ and supported Cr catalysts. A Mars-van-Krevelen kinetic model was developed based on 14 elementary steps and successfully predicted the reaction output. All catalysts exhibited excellent stability during 24- hour continuous reaction without regeneration in between. Especially, 10Fe-CeO₂ appeared to be the most stable and promising catalyst with minimal coke accumulation after 24-hour reaction test. Stability analysis revealed that Cr-related catalysts are even more stable than Fe-CeO₂ in the early 10 hours due to the dual redox circle of Ce⁽ᴵⱽ⁾/Ce⁽ᴵᴵᴵ⁾ and Fe⁽ᴵᴵᴵ⁾/Fe⁽ᴵᴵ⁾ but suffered from C-C scissoring side reactions and coke formation after 12 hours TOS.
NotePh.D.
NoteIncludes bibliographical references
Genretheses
Persistent URLhttps://doi.org/doi:10.7282/t3-r3ek-sz29
LanguageEnglish
CollectionSchool of Graduate Studies Electronic Theses and Dissertations
Organization NameRutgers, The State University of New Jersey
RightsThe author owns the copyright to this work.
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