Spatially resolved investigation into the coke formation and chemical states of nickel during autothermal reforming of acetic acid over Ni/CeO2–ZrO2 catalysts
文献情報
Nat Phongprueksathat, Thanakorn Thanasujaree, Thirasak Rirksomboon
Autothermal reforming (ATR) is a viable option for reducing coke formation and energy consumption in hydrogen production processes. The space-resolved ATR of acetic acid as a model compound over the Ni/Ce0.75Zr0.25O2 catalyst is performed using a spatial discretization approach by means of separating a reactor into up to 4 reaction zones. The spent catalysts from different zones were further characterized by ex situ XPS and TPO techniques to investigate the Ni oxidation states, coke morphology, and coke combustion. In addition, steam reforming (SR) and partial oxidation (POX) were similarly performed to decouple the effects of steam and oxygen from ATR. By comparing with SR, co-fed oxygen in ATR has significantly decreased the overall amount of coke formation with the implication on the reduced H2 yield partially due to the CO oxidation. The co-fed oxygen consumed in the frontal section of the catalyst bed resulted in the oxidation of metallic Ni, decreasing the acetic acid conversion of the initial zone of its catalyst bed. Such oxidized Ni species could also be reduced by H2 in the product stream of the previous zone resulting in a lower H2 yield. Although oxygen can reduce the overall coke formation, its coke structures have been shifted from filamentous coke to the formation of polymeric, soft, and carbidic cokes. Those types of cokes seemed to be related to the formation of NiO that promotes acetate formation and decomposition. In sum, the presence of oxygen in the part of the catalyst bed results in the differences of the catalytic activity, the oxidation state of Ni, and the pattern of coke formation; this has created two recognizable reaction zones.
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Reaction Chemistry & Engineering is an interdisciplinary journal reporting cutting-edge research focused on enhancing the understanding and efficiency of reactions. Reaction engineering leverages the interface where fundamental molecular chemistry meets chemical engineering and technology. Challenges in chemistry can be overcome by the application of new technologies, while engineers may find improved solutions for process development from the latest developments in reaction chemistry. Reaction Chemistry & Engineering is a unique forum for researchers whose interests span the broad areas of chemical engineering and chemical sciences to come together in solving problems of importance to wider society. All papers should be written to be approachable by readers across the engineering and chemical sciences. Papers that consider multiple scales, from the laboratory up to and including plant scale, are particularly encouraged.
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