Ethyl acetate abatement on copper catalysts supported on ceria doped with rare earth oxides

Sónia Alexandra Correia Carabineiro; Michalis Konsolakis; George Emmanouil Nontas Marnellos; Faizan Asad; Olívia Salomé Gonçalves Pinto Soares; Pedro Bandeira Tavares; Manuel Fernando Ribeiro Pereira; José Joaquim De Melo Órfão; José Luís Figueiredo

doi:10.3390/molecules21050644

Ethyl acetate abatement on copper catalysts supported on ceria doped with rare earth oxides

Sónia Alexandra Correia Carabineiro^*
, Michalis Konsolakis
, George Emmanouil Nontas Marnellos
, Faizan Asad
, Olívia Salomé Gonçalves Pinto Soares
, Pedro Bandeira Tavares
, Manuel Fernando Ribeiro Pereira
, José Joaquim De Melo Órfão
, José Luís Figueiredo

^*Corresponding author for this work

Not published at VTT

Universidade do Porto
Technical University of Crete
University of Western Macedonia
Centre for Research and Technology Hellas (CERTH)
University of Trás-os-Montes and Alto Douro

Research output: Contribution to journal › Article › Scientific › peer-review

41 Citations (Scopus)

Abstract

Different lanthanide (Ln)-doped cerium oxides (Ce_0.5 Ln_0.5 O_1.75, where Ln: Gd, La, Pr, Nd, Sm) were loaded with Cu (20 wt. %) and used as catalysts for the oxidation of ethyl acetate (EtOAc), a common volatile organic compound (VOC). For comparison, both Cu-free (Ce-Ln) and supported Cu (Cu/Ce-Ln) samples were characterized by N₂ adsorption at -196°C, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and temperature programmed reduction in H₂. The following activity sequence, in terms of EtOAc conversion, was found for bare supports: CeO₂ ≈ Ce_0.5Pr_0.5O_1.75 > Ce_0.5Sm_0.5O_1.75 > Ce_0.5Gd_0.5O_1.75 > Ce_0.5Nd_0.5O_1.75 > Ce_0.5La_0.5O_1.75. Cu addition improved the catalytic performance, without affecting the activity order. The best catalytic performance was obtained for Cu/CeO₂ and Cu/Ce_0.5Pr_0.5O_1.75 samples, both achieving complete EtOAc conversion below ca. 290°C. A strong correlation was revealed between the catalytic performance and the redox properties of the samples, in terms of reducibility and lattice oxygen availability. No particular correlation between the VOC oxidation performance and textural characteristics was found. The obtained results can be explained in terms of a Mars-van Krevelen type redox mechanism involving the participation of weakly bound (easily reduced) lattice oxygen and its consequent replenishment by gas phase oxygen.

Original language	English
Article number	644
Journal	Molecules
Volume	21
Issue number	5
DOIs	https://doi.org/10.3390/molecules21050644
Publication status	Published - 1 May 2016
MoE publication type	A1 Journal article-refereed

Funding

SACC thanks Funda\u00E7\u00E3o para a Ci\u00EAncia 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. OSGPS also acknowledge FCT for grant SFRH/BPD/97689/2013. This work was financially supported by Project POCI-01-0145-FEDER-006984 - Associate Laboratory LSRE-LCM funded by FEDER funds through COMPETE2020 - Programa Operacional Competitividade e Internacionaliza\u00E7\u00E3o (POCI)-and by national funds through FCT - Funda\u00E7\u00E3o para a Ci\u00EAncia e a Tecnologia. M.K. is thankful for the Greece-Portugal Bilateral Educational Program. M.F.A. is grateful for IAESTE funding (PT/2014/34). Authors are thankful to Carlos M. S\u00E1 (CEMUP) for assistance with S.E.M. and X.P.S. analyses.

Keywords

Copper (Cu)-based catalysts
Ethyl acetate oxidation
Mixed oxides
Rare earth oxides
Volatile organic compounds (VOCs)

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10.3390/molecules21050644Licence: CC BY

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title = "Ethyl acetate abatement on copper catalysts supported on ceria doped with rare earth oxides",

abstract = "Different lanthanide (Ln)-doped cerium oxides (Ce0.5 Ln0.5 O1.75, where Ln: Gd, La, Pr, Nd, Sm) were loaded with Cu (20 wt. \%) and used as catalysts for the oxidation of ethyl acetate (EtOAc), a common volatile organic compound (VOC). For comparison, both Cu-free (Ce-Ln) and supported Cu (Cu/Ce-Ln) samples were characterized by N2 adsorption at -196°C, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and temperature programmed reduction in H2. The following activity sequence, in terms of EtOAc conversion, was found for bare supports: CeO2 ≈ Ce0.5Pr0.5O1.75 > Ce0.5Sm0.5O1.75 > Ce0.5Gd0.5O1.75 > Ce0.5Nd0.5O1.75 > Ce0.5La0.5O1.75. Cu addition improved the catalytic performance, without affecting the activity order. The best catalytic performance was obtained for Cu/CeO2 and Cu/Ce0.5Pr0.5O1.75 samples, both achieving complete EtOAc conversion below ca. 290°C. A strong correlation was revealed between the catalytic performance and the redox properties of the samples, in terms of reducibility and lattice oxygen availability. No particular correlation between the VOC oxidation performance and textural characteristics was found. The obtained results can be explained in terms of a Mars-van Krevelen type redox mechanism involving the participation of weakly bound (easily reduced) lattice oxygen and its consequent replenishment by gas phase oxygen.",

keywords = "Copper (Cu)-based catalysts, Ethyl acetate oxidation, Mixed oxides, Rare earth oxides, Volatile organic compounds (VOCs)",

author = "Carabineiro, \{S{\'o}nia Alexandra Correia\} and Michalis Konsolakis and Marnellos, \{George Emmanouil Nontas\} and Faizan Asad and Soares, \{Ol{\'i}via Salom{\'e} Gon{\c c}alves Pinto\} and Tavares, \{Pedro Bandeira\} and Pereira, \{Manuel Fernando Ribeiro\} and \{De Melo {\'O}rf{\~a}o\}, \{Jos{\'e} Joaquim\} and Figueiredo, \{Jos{\'e} Lu{\'i}s\}",

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year = "2016",

month = may,

day = "1",

doi = "10.3390/molecules21050644",

language = "English",

volume = "21",

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T1 - Ethyl acetate abatement on copper catalysts supported on ceria doped with rare earth oxides

AU - Carabineiro, Sónia Alexandra Correia

AU - Konsolakis, Michalis

AU - Marnellos, George Emmanouil Nontas

AU - Asad, Faizan

AU - Soares, Olívia Salomé Gonçalves Pinto

AU - Tavares, Pedro Bandeira

AU - Pereira, Manuel Fernando Ribeiro

AU - De Melo Órfão, José Joaquim

AU - Figueiredo, José Luís

PY - 2016/5/1

Y1 - 2016/5/1

N2 - Different lanthanide (Ln)-doped cerium oxides (Ce0.5 Ln0.5 O1.75, where Ln: Gd, La, Pr, Nd, Sm) were loaded with Cu (20 wt. %) and used as catalysts for the oxidation of ethyl acetate (EtOAc), a common volatile organic compound (VOC). For comparison, both Cu-free (Ce-Ln) and supported Cu (Cu/Ce-Ln) samples were characterized by N2 adsorption at -196°C, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and temperature programmed reduction in H2. The following activity sequence, in terms of EtOAc conversion, was found for bare supports: CeO2 ≈ Ce0.5Pr0.5O1.75 > Ce0.5Sm0.5O1.75 > Ce0.5Gd0.5O1.75 > Ce0.5Nd0.5O1.75 > Ce0.5La0.5O1.75. Cu addition improved the catalytic performance, without affecting the activity order. The best catalytic performance was obtained for Cu/CeO2 and Cu/Ce0.5Pr0.5O1.75 samples, both achieving complete EtOAc conversion below ca. 290°C. A strong correlation was revealed between the catalytic performance and the redox properties of the samples, in terms of reducibility and lattice oxygen availability. No particular correlation between the VOC oxidation performance and textural characteristics was found. The obtained results can be explained in terms of a Mars-van Krevelen type redox mechanism involving the participation of weakly bound (easily reduced) lattice oxygen and its consequent replenishment by gas phase oxygen.

AB - Different lanthanide (Ln)-doped cerium oxides (Ce0.5 Ln0.5 O1.75, where Ln: Gd, La, Pr, Nd, Sm) were loaded with Cu (20 wt. %) and used as catalysts for the oxidation of ethyl acetate (EtOAc), a common volatile organic compound (VOC). For comparison, both Cu-free (Ce-Ln) and supported Cu (Cu/Ce-Ln) samples were characterized by N2 adsorption at -196°C, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy and temperature programmed reduction in H2. The following activity sequence, in terms of EtOAc conversion, was found for bare supports: CeO2 ≈ Ce0.5Pr0.5O1.75 > Ce0.5Sm0.5O1.75 > Ce0.5Gd0.5O1.75 > Ce0.5Nd0.5O1.75 > Ce0.5La0.5O1.75. Cu addition improved the catalytic performance, without affecting the activity order. The best catalytic performance was obtained for Cu/CeO2 and Cu/Ce0.5Pr0.5O1.75 samples, both achieving complete EtOAc conversion below ca. 290°C. A strong correlation was revealed between the catalytic performance and the redox properties of the samples, in terms of reducibility and lattice oxygen availability. No particular correlation between the VOC oxidation performance and textural characteristics was found. The obtained results can be explained in terms of a Mars-van Krevelen type redox mechanism involving the participation of weakly bound (easily reduced) lattice oxygen and its consequent replenishment by gas phase oxygen.

KW - Copper (Cu)-based catalysts

KW - Ethyl acetate oxidation

KW - Mixed oxides

KW - Rare earth oxides

KW - Volatile organic compounds (VOCs)

UR - https://www.scopus.com/pages/publications/84973617969

U2 - 10.3390/molecules21050644

DO - 10.3390/molecules21050644

M3 - Article

C2 - 27196886

AN - SCOPUS:84973617969

SN - 1420-3049

VL - 21

JO - Molecules

JF - Molecules

IS - 5

M1 - 644

ER -

Ethyl acetate abatement on copper catalysts supported on ceria doped with rare earth oxides

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