Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides

M. Konsolakis; S. A.C. Carabineiro; G. E. Marnellos; M. F. Asad; O. S.G.P. Soares; M. F.R. Pereira; J. J.M. Órfão; J. L. Figueiredo

doi:10.1016/j.jcis.2017.02.014

Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides

M. Konsolakis, S. A.C. Carabineiro^*, G. E. Marnellos, M. F. Asad, O. S.G.P. Soares, M. F.R. Pereira, J. J.M. Órfão, J. L. Figueiredo

^*Corresponding author for this work

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Abstract

Cobalt-cerium mixed oxides were prepared by the wet impregnation method and evaluated for volatile organic compounds (VOCs) abatement, using ethyl acetate (EtAc) as model molecule. The impact of Co content on the physicochemical characteristics of catalysts and EtAc conversion was investigated. The materials were characterized by various techniques, including N₂ adsorption at −196 °C, scanning electron microscopy (SEM), X-ray diffraction (XRD), H₂-temperature programmed reduction (H₂-TPR) and X-ray photoelectron spectroscopy (XPS) to reveal the structure–activity relationship. The obtained results showed the superiority of mixed oxides compared to bare CeO₂ and Co₃O₄, demonstrating a synergistic effect. The optimum oxidation performance was achieved with the sample containing 20 wt.% Co (Co/Ce atomic ratio of ca. 0.75), in which complete conversion of EtAc was attained at 260 °C. In contrast, temperatures above 300 °C were required to achieve 100% conversion over the single oxides. Notably, a strong relationship between both the: (i) relative population, and (ii) facile reduction of lattice oxygen with the ethyl acetate oxidation activity was found, highlighting the key role of loosely bound oxygen species on VOCs oxidation. A synergistic Co-Ce interaction can be accounted for the enhanced reducibility of mixed oxides, linked with the increased mobility of lattice oxygen.

Original language	English
Pages (from-to)	141-149
Number of pages	9
Journal	Journal of Colloid and Interface Science
Volume	496
DOIs	https://doi.org/10.1016/j.jcis.2017.02.014
Publication status	Published - 15 Jun 2017
MoE publication type	A1 Journal article-refereed

Funding

SACC thanks Fundação para a Ciência e Tecnologia (FCT) for financial support, including Investigador FCT program (IF/01381/2013/CP1160/CT0007), with financing from the European Social Fund and the Human Potential Operational Program. This work is a result of project “AIProcMat@N2020 – Advanced Industrial Processes and Materials for a Sustainable Northern Region of Portugal 2020”, with the reference NORTE-01-0145-FEDER-000006, supported by Norte Portugal Regional Operational Programme (NORTE 2020), under the Portugal 2020 Partnership Agreement, through the European Regional Development Fund (ERDF) and of Project POCI-01-0145-FEDER-006984 – Associate Laboratory LSRE-LCM funded by ERDF through COMPETE2020 - Programa Operacional Competitividade e Internacionalização (POCI) – and by national funds through FCT - Fundação para a Ciência e a Tecnologia. MK is thankful for the Greece–Portugal Bilateral Educational Program. MFA is grateful for IAESTE funding (PT/2014/34). Authors are thankful to Dr. Carlos M. Sá (CEMUP) for assistance with SEM and XPS analyses.

Keywords

CeO
CoO
Cobalt (Co)-based catalysts
Ethyl acetate oxidation
Volatile organic compounds (VOCs)

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Konsolakis, M., Carabineiro, S. A. C., Marnellos, G. E., Asad, M. F., Soares, O. S. G. P., Pereira, M. F. R., Órfão, J. J. M., & Figueiredo, J. L. (2017). Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides. Journal of Colloid and Interface Science, 496, 141-149. https://doi.org/10.1016/j.jcis.2017.02.014

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title = "Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides",

abstract = "Cobalt-cerium mixed oxides were prepared by the wet impregnation method and evaluated for volatile organic compounds (VOCs) abatement, using ethyl acetate (EtAc) as model molecule. The impact of Co content on the physicochemical characteristics of catalysts and EtAc conversion was investigated. The materials were characterized by various techniques, including N2 adsorption at −196 °C, scanning electron microscopy (SEM), X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) to reveal the structure–activity relationship. The obtained results showed the superiority of mixed oxides compared to bare CeO2 and Co3O4, demonstrating a synergistic effect. The optimum oxidation performance was achieved with the sample containing 20 wt.\% Co (Co/Ce atomic ratio of ca. 0.75), in which complete conversion of EtAc was attained at 260 °C. In contrast, temperatures above 300 °C were required to achieve 100\% conversion over the single oxides. Notably, a strong relationship between both the: (i) relative population, and (ii) facile reduction of lattice oxygen with the ethyl acetate oxidation activity was found, highlighting the key role of loosely bound oxygen species on VOCs oxidation. A synergistic Co-Ce interaction can be accounted for the enhanced reducibility of mixed oxides, linked with the increased mobility of lattice oxygen.",

keywords = "CeO, CoO, Cobalt (Co)-based catalysts, Ethyl acetate oxidation, Volatile organic compounds (VOCs)",

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year = "2017",

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doi = "10.1016/j.jcis.2017.02.014",

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T1 - Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides

AU - Konsolakis, M.

AU - Carabineiro, S. A.C.

AU - Marnellos, G. E.

AU - Asad, M. F.

AU - Soares, O. S.G.P.

AU - Pereira, M. F.R.

AU - Órfão, J. J.M.

AU - Figueiredo, J. L.

PY - 2017/6/15

Y1 - 2017/6/15

N2 - Cobalt-cerium mixed oxides were prepared by the wet impregnation method and evaluated for volatile organic compounds (VOCs) abatement, using ethyl acetate (EtAc) as model molecule. The impact of Co content on the physicochemical characteristics of catalysts and EtAc conversion was investigated. The materials were characterized by various techniques, including N2 adsorption at −196 °C, scanning electron microscopy (SEM), X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) to reveal the structure–activity relationship. The obtained results showed the superiority of mixed oxides compared to bare CeO2 and Co3O4, demonstrating a synergistic effect. The optimum oxidation performance was achieved with the sample containing 20 wt.% Co (Co/Ce atomic ratio of ca. 0.75), in which complete conversion of EtAc was attained at 260 °C. In contrast, temperatures above 300 °C were required to achieve 100% conversion over the single oxides. Notably, a strong relationship between both the: (i) relative population, and (ii) facile reduction of lattice oxygen with the ethyl acetate oxidation activity was found, highlighting the key role of loosely bound oxygen species on VOCs oxidation. A synergistic Co-Ce interaction can be accounted for the enhanced reducibility of mixed oxides, linked with the increased mobility of lattice oxygen.

AB - Cobalt-cerium mixed oxides were prepared by the wet impregnation method and evaluated for volatile organic compounds (VOCs) abatement, using ethyl acetate (EtAc) as model molecule. The impact of Co content on the physicochemical characteristics of catalysts and EtAc conversion was investigated. The materials were characterized by various techniques, including N2 adsorption at −196 °C, scanning electron microscopy (SEM), X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) to reveal the structure–activity relationship. The obtained results showed the superiority of mixed oxides compared to bare CeO2 and Co3O4, demonstrating a synergistic effect. The optimum oxidation performance was achieved with the sample containing 20 wt.% Co (Co/Ce atomic ratio of ca. 0.75), in which complete conversion of EtAc was attained at 260 °C. In contrast, temperatures above 300 °C were required to achieve 100% conversion over the single oxides. Notably, a strong relationship between both the: (i) relative population, and (ii) facile reduction of lattice oxygen with the ethyl acetate oxidation activity was found, highlighting the key role of loosely bound oxygen species on VOCs oxidation. A synergistic Co-Ce interaction can be accounted for the enhanced reducibility of mixed oxides, linked with the increased mobility of lattice oxygen.

KW - CeO

KW - CoO

KW - Cobalt (Co)-based catalysts

KW - Ethyl acetate oxidation

KW - Volatile organic compounds (VOCs)

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JO - Journal of Colloid and Interface Science

JF - Journal of Colloid and Interface Science

ER -

Effect of cobalt loading on the solid state properties and ethyl acetate oxidation performance of cobalt-cerium mixed oxides

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