MnOx/ZrO2‒CeO2 catalysts for CO and propane oxidation: The effect of manganese content

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Abstract

The effect of the content of supported manganese on the structural properties and activity in the oxidation reactions of CO and propane for the MnОx/Zr0.4Ce0.6 catalysts prepared by the impregnation method has been studied. It was found that an increase in manganese content to 3.6% wt. (molar ratio Mn/(Zr + Ce) ≤ 0.1) leads to an increase in the catalytic activity of MnОx/Zr0.4Ce0.6 in oxidation reactions. In the case of a higher manganese concentration, the activity changes slightly. According to the XRD, TPR-H2, XPS and EPR, an increase in the amount of supported manganese for samples with Mn/(Zr + Ce) ≤ 0.1 is accompanied by a change in the lattice constant of the support, an increase in the amount of weakly bound oxygen, as well as the quantity of oxygen vacancies in the structure of cerium oxide. These changes are due to the incorporation of manganese into the structure of the support and the possible formation of highly dispersed particles of MnОx on its surface which ensures an increase in catalytic activity. Stabilization of catalytic activity with a further increase in the amount of supported manganese correlates with a slight change in the amount of weakly bound oxygen and oxygen vacancies of the support due to the appearance and subsequent increase in the content of the less active Mn2O3 phase.

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About the authors

T. N. Afonasenko

Institute of Catalysis SB RAS

Author for correspondence.
Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

D. V. Yurpalova

Institute of Catalysis SB RAS

Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

V. L. Yurpalov

Center of New Chemical Technologies, Boreskov Institute of Catalysis SB RAS

Email: atnik@ihcp.ru
Russian Federation, Neftezavodskaya, 54, Omsk, 644040

V. P. Konovalova

Institute of Catalysis SB RAS

Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

V. A. Rogov

Institute of Catalysis SB RAS

Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

E. E. Aydakov

Institute of Catalysis SB RAS; Synchrotron Radiation Facility SKIF, Boreskov Institute of Catalysis SB RA

Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090; Nikolsky Prosp., 1, Kol’tsovo, 630559

A. N. Serkova

Institute of Catalysis SB RAS

Email: atnik@ihcp.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

O. A. Bulavchenko

Institute of Catalysis SB RAS

Email: obulavchenko@catalysis.ru
Russian Federation, Lavrentiev Ave., 5, Novosibirsk, 630090

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Supplementary files

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2. Fig. 1. CO conversion as a function of temperature in the oxidation reaction in the presence of Mnx/Zr0.4Ce0.6 catalysts with different manganese content. Inset: temperature of 50% CO conversion depending on the Mn/(Zr + Ce) ratio.

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3. Fig. 2. Propane conversion as a function of temperature in the oxidation reaction in the presence of Mnx/Zr0.4Ce0.6 catalysts with different manganese content. Inset: temperature of 50% propane conversion depending on the Mn/(Zr + Ce) ratio.

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4. Fig. 3. XRD patterns of Mnx/Zr0.4Ce0.6 samples with different manganese content.

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5. Fig. 4. H2-TPR profiles of Mnx/Zr0.4Ce0.6 samples.

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6. Fig. 5. EPR spectra of samples Mn0.025/Zr0.4Ce0.6 (1), Mn0.05/Zr0.4Ce0.6 (2), Mn0.1/Zr0.4Ce0.6 (3), and Mn0.2/Zr0.4Ce0.6 (4).

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7. Fig. 6. SEM data of samples Mn0.05/Zr0.4Ce0.6 (a, b), Mn0.1/Zr0.4Ce0.6 (c, d), and Mn0.3/Zr0.4Ce0.6 (e, f).

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8. Fig. 7. XPS spectra Ce3d (a) and Mn2p (b) of Mnx/Zr0.4Ce0.6 samples with different manganese content.

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