Effect of manganese or copper on catalytic properties of CeO2-SiO2 in the preferential oxidation of CO in excess of hydrogen (PROX-СО)

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Resumo

The work is directed to identifying the effect of copper or manganese oxide additives on the catalytic properties of the CeO2–SiO2 (CeSi) system containing silicon dioxide as a textural promoter in the preferential oxidation of carbon monoxide in excess hydrogen (PROX-CO). The CeSi catalyst was prepared by precipitation from salts in the presence of cetyltrimethylammonium bromide template, 5 wt % MnOx/CeSi and 5 wt % CuOх/CeSi were obtained by precipitation of modifiers from salts in the presence of potassium carbonate. The catalytic efficiency in PROX-CO increases in the series CeSi > Mn/CeSi > Cu/CeSi (at 200°C the time-averaged CO conversion values are 5, 19 and 78%, CO2 selectivity values are 100, 65 and 59%). Characterization by X-ray diffraction, scanning electron microscopy, low-temperature nitrogen adsorption-desorption, Raman spectroscopy, X-ray photoelectron spectroscopy and temperature-programmed reduction with hydrogen demonstrated, that the presence of SiO2 promotes the formation of highly dispersed and easily reduced CuOx clusters in close contact with CeO2 particles, uniformly distributed over CeSi, and containing Cu+ adsorption centers. The Mn/CeSi system is characterized by an uneven distribution of manganese on the surface, a low number of MnOx-CeO2 contacts, and a low reduction ability of MnOx in the low-temperature range (50–100°C).

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Sobre autores

I. Kaplin

Lomonosov Moscow State University

Autor responsável pela correspondência
Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0002-5091-6290

PhD, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

E. Boltkov

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com

student, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

L. Efimenko

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com

student, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

E. Lokteva

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0003-3510-4822

Doctor of Chemical Sciences, Associate Professor, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

O. Isaikina

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0002-4165-6562

PhD, Associate Professor, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

K. Maslakov

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0002-0672-2683

PhD, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

A. Kamaev

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0002-6648-0647

Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

E. Golubina

Lomonosov Moscow State University

Email: kaplinigormsu@gmail.com
ORCID ID: 0000-0002-1040-1428

Doctor of Chemical Sciences, Associate Professor, Chemistry Department

Rússia, Leninskie Gory, 1, building 3, Moscow, 119991

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2. Fig. 1. Dependences of the conversion of carbon monoxide (X(CO)) and oxygen (X(O2)), selectivity for carbon dioxide calculated from the loss of CO (S1(CO2)) and the formation of CO2 (S2(CO2), on the reaction temperature and time in the flow of the reaction mixture (a–c) and the contact time (d–e) in the presence of CeSi (a, d), Mn/CeSi (b, d) and Cu/CeSi (c, f) samples.

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3. Fig. 2. Powder diffraction patterns of freshly prepared CeSi, Cu/CeSi and Mn/CeSi samples.

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4. Fig. 3. SEM micrographs (a, c) and EDA maps of the distribution of manganese (b) and copper (d) on the surface of Mn/CeSi (a, b) and Cu/CeSi (c, d) catalysts.

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5. Rice. 4. Raman spectra (a) and TPR-H2 profiles (b) of CeSi, Cu/CeSi and Mn/CeSi samples.

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