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Surface Engineering of CeO2 Catalysts: Differences Between Solid Solution Based and Interfacially Designed Ce1−xMxO2 and MO/CeO2 (M = Zn, Mn) in CO2 Hydrogenation Reaction

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Abstract

Zn- and Mn-doped Cerium-oxide based catalyst textured as a solid solutional as well as interfacial form was compared in CO2 hydrogenation reaction to understand the role of texture as well as dopant type. Ce0.9M0.1O2 (M = Zn, Mn) solid solution was prepared by hydrothermal method and CeO2 supported 10 mol% metal oxide (Metal = Zn, Mn) were prepared by wet impregnation method, where the catalysts were characterized by XRD, N2 adsorption/desorption isotherm, TEM, Raman spectra, HAADF-STEM and H2-TPR. During the CO2 activation reaction, CO was the major product with minor amounts of methane, ethane, methanol and ethanol. In the case of the Zn-doped CeO2 catalyst, the presence of Zn improved catalytic activity in both solid solutional and interfacial form due to the synergetic effect of Zn-Ce-based oxide. However, for MnOx/CeO2 catalysts, the CO2 consumption rate significantly decreased for 10 mol% MnOx/CeO2, Ce0.9Mn0.1O2 and Mn3O4, where the MnOx addition inhibits the reduction of CeO2. In the case of the pure CeO2, DRIFTS spectra show that formate intermediate formed by reaction between activated CO2 and OH transformed into methoxy species through formaldehyde intermediates, which leads to the formation of small amount of methanol and ethanol.

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Acknowledgement

AS gratefully acknowledges the support of the Bolyai Janos Research Fellowship of the Hungarian Academy of Science and the “UNKP-20-5-SZTE-663” New National Excellence Program of the Ministry for Innovation and Technology from the source of the National Research, Development and Innovation Fund. ISZ grateful for the fund of UNKP-20-4-SZTE-634 New National Excellence Program of the Ministry for Innovation and Technology The financial support of the Hungarian National Research, Development and Innovation Office through the GINOP-2.3.2-15-2016-00013 project "Intelligent materials based on functional surfaces—from syntheses to applications" and the Ministry of Human Capacities through the EFOP-3.6.1-16-2016-00014 project and the 20391-3/2018/FEKUSTRAT are acknowledged.

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  1. Department of Applied and Environmental Chemistry, Interdisciplinary Excellence Centre, University of Szeged, Rerrich Béla tér 1, Szeged, 6720, Hungary

    T. Rajkumar, András Sápi, Marietta Ábel, János Kiss, Imre Szenti, Kornélia Baán, Juan Fernando Gómez-Pérez, Ákos Kukovecz & Zoltán Kónya

  2. Institute of Environmental and Technological Sciences, University of Szeged, Szeged, 6720, Hungary

    András Sápi

  3. MTA-SZTE Reaction Kinetics and Surface Chemistry Research Group, University of Szeged, Rerrich Béla tér 1, Szeged, 6720, Hungary

    János Kiss, Imre Szenti & Zoltán Kónya

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Rajkumar, T., Sápi, A., Ábel, M. et al. Surface Engineering of CeO2 Catalysts: Differences Between Solid Solution Based and Interfacially Designed Ce1−xMxO2 and MO/CeO2 (M = Zn, Mn) in CO2 Hydrogenation Reaction. Catal Lett 151, 3477–3491 (2021). https://doi.org/10.1007/s10562-021-03591-y

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