Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator

The deactivation of supported nickel catalysts by coking is an important technological subject for many chemical processes, especially when high concentrations of unsaturated hydrocarbons are present in the feed gas. Here, the reversible segregation of Ni from a LaFeO 3 AE d perovskite-type host lattice was exploited to completely recover a LaFe 0.8 Ni 0.2 O 3 AE d catalyst after it had been deliberately subjected to severe carbon deposition during CO 2 methanation in ethylene rich feed gas for several hours. Temperature programmed reduction, X-ray diffraction, electron microscopy, X-ray absorption spectroscopy and catalytic activity tests were used to follow the catalyst structure along the various steps of reduction, reaction, coking and subsequent regeneration, while Raman spectroscopy and electron microscopy were used to characterize the nature of the carbon deposits. It is shown that upon reduction Ni atoms segregate to the surface of the perovskite to form catalytic active Ni particles. Oxidation stimulates Ni atoms to readopt the coordination environment of Fe in the perovskite matrix. This property persisted after severe catalyst deactivation by filamentous, partially graphitic carbon. It is demonstrated that simple catalyst reoxidation can be applied to oxidize all carbon deposits while additionally reverting segregated Ni back into the host lattice, thus protecting Ni from particle growth and resultant long-term loss of catalyst activity over multiple regeneration cycles.

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Reversible Segregation of Ni in LaFe_0.8Ni_0.2O_3±δ During Coke Removal

Steiger

Nachtegaal

Kröcher

et al. 2018

ChemCatChem

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Methane Combustion Over Ni/Ce_xZr_1–xO₂ Catalysts: Impact of Ceria/Zirconia Ratio

et al. 2020

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A series of CexZr1–xO2 (x=1, 0.83, 0.17, 0) supports and 2 wt.% Ni/CexZr1–xO2 catalysts were synthesized and evaluated for CH4 oxidation. The CexZr1–xO2 supports showed moderate activity (T50=519‐638 °C) with CO by‐product formation. Nickel incorporation onto CexZr1–xO2 lowered the T50 to 438–477 °C and eliminated the formation of CO. The results indicated that moderate Zr doping improved the support oxygen storage capacity (OSC) and reducibility of the catalyst at low temperatures (H2‐TPR) leading to an enhanced CH4 combustion turnover frequency: Ni/ZrO2

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Interfacial CoO_x Layers on TiO₂ as an Efficient Catalyst for Solvent‐Free Aerobic Oxidation of Hydrocarbons

Wang

Zhang

et al. 2018

ChemSusChem

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Construction of efficient interfaces to improve the performance of supported metal catalysts is a challenging but effective technique. A newly synthesized catalyst with layered cobalt oxide on the surface of titania (layer‐CoOx/TiO2) is highly selective towards the aerobic oxidation of C−H bonds in a series of hydrocarbons under sustainable conditions. The layer‐CoOx/TiO2 easily outperforms the state‐of‐the‐art noble metal catalysts and homogeneous cobalt salts used in industry. In‐depth structural and functional characterization reveal that the layer‐CoOx/TiO2 readily reacts with O2 for the adsorption and activation of C−H bonds. The layered structure of CoOx can maximize the interfacial effect of CoOx/TiO2 leading to a good performance for the oxidation of C−H bonds.

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Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator

Cited by 3 publications

References 42 publications

Reversible Segregation of Ni in LaFe_0.8Ni_0.2O_3±δ During Coke Removal

Reversible Segregation of Ni in LaFe_0.8Ni_0.2O_3±δ During Coke Removal

Methane Combustion Over Ni/Ce_xZr_1–xO₂ Catalysts: Impact of Ceria/Zirconia Ratio

Interfacial CoO_x Layers on TiO₂ as an Efficient Catalyst for Solvent‐Free Aerobic Oxidation of Hydrocarbons

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Produktion von Methanol und Ethanol aus Methan in einem einzigen Reaktor mit einem Nickeloxid auf Ceroxid‐Zirconiumoxid‐Katalysator

Cited by 3 publications

References 42 publications

Reversible Segregation of Ni in LaFe0.8Ni0.2O3±δ During Coke Removal

Reversible Segregation of Ni in LaFe0.8Ni0.2O3±δ During Coke Removal

Methane Combustion Over Ni/CexZr1–xO2 Catalysts: Impact of Ceria/Zirconia Ratio

Interfacial CoOx Layers on TiO2 as an Efficient Catalyst for Solvent‐Free Aerobic Oxidation of Hydrocarbons

Contact Info

Product

Resources

About

Reversible Segregation of Ni in LaFe_0.8Ni_0.2O_3±δ During Coke Removal

Reversible Segregation of Ni in LaFe_0.8Ni_0.2O_3±δ During Coke Removal

Methane Combustion Over Ni/Ce_xZr_1–xO₂ Catalysts: Impact of Ceria/Zirconia Ratio

Interfacial CoO_x Layers on TiO₂ as an Efficient Catalyst for Solvent‐Free Aerobic Oxidation of Hydrocarbons