Insight into CO2 methanation mechanism over NiUSY zeolites: An operando IR study

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

doi:10.1016/j.apcatb.2015.02.026

Insight into CO₂ methanation mechanism over NiUSY zeolites: An operando IR 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

219 Citations (Scopus)

Abstract

Ni-impregnated USY zeolites with increasing Ni content (5, 10, 14%_wt.) were investigated by operando IR spectroscopy for both CO₂ adsorption and CO₂ methanation conditions reaction. In-situ FTIR and TPD experiments highlighted a rather weak CO₂ adsorption, which occurs namely as carbonates or CO₂ linear complexes over cations (e.g., Na⁺). Under methanation conditions, dissociated hydrogen reacts with carbonates and/or physisorbed CO₂, leading to monodentate formates, then carbonyls (both adsorbed onto Ni⁰ particles), and finally to methane. A detailed mechanism of the pathways involved in CO₂ methanation over NiUSY catalysts is then discussed in accordance with infrared spectroscopic data.

Original language	English
Pages (from-to)	120-125
Number of pages	6
Journal	Applied Catalysis B: Environmental
Volume	174-175
DOIs	https://doi.org/10.1016/j.apcatb.2015.02.026
Publication status	Published - 1 Sept 2015

Bibliographical note

Acknowledgements
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

Carbonyls
Formates
Infrared operando spectroscopy
Mechanism
Ni-based zeolite

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10.1016/j.apcatb.2015.02.026Licence: Unspecified

Cite this

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title = "Insight into CO2 methanation mechanism over NiUSY zeolites: An operando IR study",

abstract = "Ni-impregnated USY zeolites with increasing Ni content (5, 10, 14%wt.) were investigated by operando IR spectroscopy for both CO2 adsorption and CO2 methanation conditions reaction. In-situ FTIR and TPD experiments highlighted a rather weak CO2 adsorption, which occurs namely as carbonates or CO2 linear complexes over cations (e.g., Na+). Under methanation conditions, dissociated hydrogen reacts with carbonates and/or physisorbed CO2, leading to monodentate formates, then carbonyls (both adsorbed onto Ni0 particles), and finally to methane. A detailed mechanism of the pathways involved in CO2 methanation over NiUSY catalysts is then discussed in accordance with infrared spectroscopic data.",

keywords = "Carbonyls, Formates, Infrared operando spectroscopy, Mechanism, Ni-based zeolite",

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 = "Acknowledgements 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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doi = "10.1016/j.apcatb.2015.02.026",

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T2 - An operando IR 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 - Acknowledgements 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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N2 - Ni-impregnated USY zeolites with increasing Ni content (5, 10, 14%wt.) were investigated by operando IR spectroscopy for both CO2 adsorption and CO2 methanation conditions reaction. In-situ FTIR and TPD experiments highlighted a rather weak CO2 adsorption, which occurs namely as carbonates or CO2 linear complexes over cations (e.g., Na+). Under methanation conditions, dissociated hydrogen reacts with carbonates and/or physisorbed CO2, leading to monodentate formates, then carbonyls (both adsorbed onto Ni0 particles), and finally to methane. A detailed mechanism of the pathways involved in CO2 methanation over NiUSY catalysts is then discussed in accordance with infrared spectroscopic data.

AB - Ni-impregnated USY zeolites with increasing Ni content (5, 10, 14%wt.) were investigated by operando IR spectroscopy for both CO2 adsorption and CO2 methanation conditions reaction. In-situ FTIR and TPD experiments highlighted a rather weak CO2 adsorption, which occurs namely as carbonates or CO2 linear complexes over cations (e.g., Na+). Under methanation conditions, dissociated hydrogen reacts with carbonates and/or physisorbed CO2, leading to monodentate formates, then carbonyls (both adsorbed onto Ni0 particles), and finally to methane. A detailed mechanism of the pathways involved in CO2 methanation over NiUSY catalysts is then discussed in accordance with infrared spectroscopic data.

KW - Carbonyls

KW - Formates

KW - Infrared operando spectroscopy

KW - Mechanism

KW - Ni-based zeolite

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VL - 174-175

SP - 120

EP - 125

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

ER -

Insight into CO₂ methanation mechanism over NiUSY zeolites: An operando IR study

Abstract

Bibliographical note

Keywords

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Ines Biscaya Semedo Pereira da Graca

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Insight into CO2 methanation mechanism over NiUSY zeolites: An operando IR study

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Bibliographical note

Keywords

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Ines Biscaya Semedo Pereira da Graca

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Insight into CO₂ methanation mechanism over NiUSY zeolites: An operando IR study