The promoting effect of Ce in the CO
                        2
                        methanation performances on NiUSY zeolite: A FTIR In Situ/Operando study

A. Westermann; B. Azambre; M. C. Bacariza; I. Graça; M. F. Ribeiro; J. M. Lopes; C. Henriques

doi:10.1016/j.cattod.2016.02.031

The promoting effect of Ce in the CO ₂ methanation performances on NiUSY zeolite: A FTIR In Situ/Operando study

A. Westermann^*, B. Azambre, M. C. Bacariza, I. Graça, M. F. Ribeiro, J. M. Lopes, C. Henriques

^*Corresponding author for this work

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

90 Citations (Scopus)

Abstract

The behavior of 5% _wt. Ni-impregnated and 5% _wt. Ni-15% _wt. Ce-impregnated zeolites (of USY type) were investigated by in situ/operando IR spectroscopy, both for CO ₂ adsorption and under methanation conditions (H ₂ :CO ₂ /4:1) reaction. In situ FTIR and CO ₂ -TPD experiments highlighted that CO ₂ adsorption is rather poor over NiUSY zeolite, whereas CO ₂ uptake over CeNiUSY leads to the formation of a large amount of adsorbed carbonates on the CeO ₂ surface. Mechanistic pathways involved in CO ₂ methanation over CeNiUSY catalyst are discussed in accordance with infrared spectroscopic data. Under methanation conditions, hydrogen is dissociated on Ni° particles and reacts with hydrogen and bidentate carbonates, leading first to the formation of monodentate formates, and then to methane, by further hydrogenation. No adsorbed carbonyls onto Ni° were detected while a large amount of formates was highlighted from 150 °C. The formate decomposition appears to be a kinetic relevant step to the observed kinetics of the CO ₂ hydrogenation reaction.

Original language	English
Pages (from-to)	74-81
Number of pages	8
Journal	Catalysis Today
Volume	283
Early online date	12 Mar 2016
DOIs	https://doi.org/10.1016/j.cattod.2016.02.031
Publication status	Published - 1 Apr 2017

Bibliographical note

This work was supported by the Framework 7 program, under the project CEOPS-CO2-loop for energy storage and conversion to organic chemistry processes through advanced catalytic systems (FP7-NMP-2012-309984).

Keywords

Carbonates
Ce–Ni-based zeolite
Formates
FTIR spectroscopy
Methane

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Cite this

@article{21d1aee12a4641389cd32ef788ff502c,

title = "The promoting effect of Ce in the CO 2 methanation performances on NiUSY zeolite: A FTIR In Situ/Operando study",

abstract = " The behavior of 5% wt. Ni-impregnated and 5% wt. Ni-15% wt. Ce-impregnated zeolites (of USY type) were investigated by in situ/operando IR spectroscopy, both for CO 2 adsorption and under methanation conditions (H 2 :CO 2 /4:1) reaction. In situ FTIR and CO 2 -TPD experiments highlighted that CO 2 adsorption is rather poor over NiUSY zeolite, whereas CO 2 uptake over CeNiUSY leads to the formation of a large amount of adsorbed carbonates on the CeO 2 surface. Mechanistic pathways involved in CO 2 methanation over CeNiUSY catalyst are discussed in accordance with infrared spectroscopic data. Under methanation conditions, hydrogen is dissociated on Ni° particles and reacts with hydrogen and bidentate carbonates, leading first to the formation of monodentate formates, and then to methane, by further hydrogenation. No adsorbed carbonyls onto Ni° were detected while a large amount of formates was highlighted from 150 °C. The formate decomposition appears to be a kinetic relevant step to the observed kinetics of the CO 2 hydrogenation reaction. ",

keywords = "Carbonates, Ce–Ni-based zeolite, Formates, FTIR spectroscopy, Methane",

author = "A. Westermann and B. Azambre and Bacariza, {M. C.} and I. Gra{\c c}a and Ribeiro, {M. F.} and Lopes, {J. M.} and C. Henriques",

note = "This work was supported by the Framework 7 program, under the project CEOPS-CO2-loop for energy storage and conversion to organic chemistry processes through advanced catalytic systems (FP7-NMP-2012-309984).",

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T2 - A FTIR In Situ/Operando study

AU - Westermann, A.

AU - Azambre, B.

AU - Bacariza, M. C.

AU - Graça, I.

AU - Ribeiro, M. F.

AU - Lopes, J. M.

AU - Henriques, C.

N1 - This work was supported by the Framework 7 program, under the project CEOPS-CO2-loop for energy storage and conversion to organic chemistry processes through advanced catalytic systems (FP7-NMP-2012-309984).

PY - 2017/4/1

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N2 - The behavior of 5% wt. Ni-impregnated and 5% wt. Ni-15% wt. Ce-impregnated zeolites (of USY type) were investigated by in situ/operando IR spectroscopy, both for CO 2 adsorption and under methanation conditions (H 2 :CO 2 /4:1) reaction. In situ FTIR and CO 2 -TPD experiments highlighted that CO 2 adsorption is rather poor over NiUSY zeolite, whereas CO 2 uptake over CeNiUSY leads to the formation of a large amount of adsorbed carbonates on the CeO 2 surface. Mechanistic pathways involved in CO 2 methanation over CeNiUSY catalyst are discussed in accordance with infrared spectroscopic data. Under methanation conditions, hydrogen is dissociated on Ni° particles and reacts with hydrogen and bidentate carbonates, leading first to the formation of monodentate formates, and then to methane, by further hydrogenation. No adsorbed carbonyls onto Ni° were detected while a large amount of formates was highlighted from 150 °C. The formate decomposition appears to be a kinetic relevant step to the observed kinetics of the CO 2 hydrogenation reaction.

AB - The behavior of 5% wt. Ni-impregnated and 5% wt. Ni-15% wt. Ce-impregnated zeolites (of USY type) were investigated by in situ/operando IR spectroscopy, both for CO 2 adsorption and under methanation conditions (H 2 :CO 2 /4:1) reaction. In situ FTIR and CO 2 -TPD experiments highlighted that CO 2 adsorption is rather poor over NiUSY zeolite, whereas CO 2 uptake over CeNiUSY leads to the formation of a large amount of adsorbed carbonates on the CeO 2 surface. Mechanistic pathways involved in CO 2 methanation over CeNiUSY catalyst are discussed in accordance with infrared spectroscopic data. Under methanation conditions, hydrogen is dissociated on Ni° particles and reacts with hydrogen and bidentate carbonates, leading first to the formation of monodentate formates, and then to methane, by further hydrogenation. No adsorbed carbonyls onto Ni° were detected while a large amount of formates was highlighted from 150 °C. The formate decomposition appears to be a kinetic relevant step to the observed kinetics of the CO 2 hydrogenation reaction.

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