Magnesium as promoter of CO2 methanation on Ni-based USY zeolites

Maria C. Bacariza, Inês Graça, Suse S. Bebiano, José M. Lopes, Carlos Henriques

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

CO2 methanation was studied over Ni–Mg–USY zeolite catalysts. Mg was added by incipient wetness impregnation and ion exchange. Whatever the Mg incorporation method used, Mg is able to improve the performance of the Ni-zeolite catalysts. Magnesium impregnation at lower contents (below 2.5%) over a 5%Ni/zeolite leads to an enhancement of the CO2 conversion into methane of 15% at 350–450 °C, probably due to the induced increase of the Ni particle dispersion, as well as to the possible activation of CO2 on the defects present on the MgO surface. At higher Mg contents, the stronger interaction between Ni and Mg oxides, leading to the formation of NiO–MgO solid solutions, seems to reduce the reducibility of the Ni species, decreasing the amount of nickel active sites available and thus the catalytic performance. Furthermore, important improvements of the catalytic performance (CO2 conversion and CH4 selectivity increased around 20% at 350–450 °C) were also found for the Mg-exchanged 5%Ni/zeolite. The results are comparable to those obtained by impregnation, but lower Mg contents are required. The enhanced activation of CO2 on Mg2+, the more dispersed Ni particles on the support, as well as the enhanced Ni reducibility when compared to the impregnated catalysts can explain the observed results. The beneficial effect of the Mg addition both by impregnation and ion exchange was also observed for samples containing higher amounts of Ni, the best sample remaining stable after 10 h under reaction conditions. Thus, Mg could be an interesting promoter for CO2 methanation over Ni-zeolite catalysts.
LanguageEnglish
Pages9776–9789
Number of pages14
JournalEnergy and Fuels
Volume31
Issue number9
Early online date28 Jul 2017
DOIs
Publication statusPublished - 21 Sep 2017

Fingerprint

Methanation
Zeolites
Impregnation
Magnesium
Catalysts
Ion exchange
Chemical activation
Methane
Solid solutions
Nickel
Oxides
Defects

Keywords

  • CO2 methanation
  • Ni–Mg–USY zeolite catalysts
  • ion exchange
  • oxides
  • catalytic performance

Cite this

Bacariza, M. C., Graça, I., Bebiano, S. S., Lopes, J. M., & Henriques, C. (2017). Magnesium as promoter of CO2 methanation on Ni-based USY zeolites. Energy and Fuels, 31(9), 9776–9789. https://doi.org/10.1021/acs.energyfuels.7b01553
Bacariza, Maria C. ; Graça, Inês ; Bebiano, Suse S. ; Lopes, José M. ; Henriques, Carlos. / Magnesium as promoter of CO2 methanation on Ni-based USY zeolites. In: Energy and Fuels. 2017 ; Vol. 31, No. 9. pp. 9776–9789.
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Bacariza, MC, Graça, I, Bebiano, SS, Lopes, JM & Henriques, C 2017, 'Magnesium as promoter of CO2 methanation on Ni-based USY zeolites' Energy and Fuels, vol. 31, no. 9, pp. 9776–9789. https://doi.org/10.1021/acs.energyfuels.7b01553

Magnesium as promoter of CO2 methanation on Ni-based USY zeolites. / Bacariza, Maria C.; Graça, Inês; Bebiano, Suse S.; Lopes, José M. ; Henriques, Carlos.

In: Energy and Fuels, Vol. 31, No. 9, 21.09.2017, p. 9776–9789.

Research output: Contribution to journalArticle

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T1 - Magnesium as promoter of CO2 methanation on Ni-based USY zeolites

AU - Bacariza, Maria C.

AU - Graça, Inês

AU - Bebiano, Suse S.

AU - Lopes, José M.

AU - Henriques, Carlos

N1 - This document is the Accepted Manuscript version of a Published Work that appeared in final form in Energy & Fuels, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.energyfuels.7b01553

PY - 2017/9/21

Y1 - 2017/9/21

N2 - CO2 methanation was studied over Ni–Mg–USY zeolite catalysts. Mg was added by incipient wetness impregnation and ion exchange. Whatever the Mg incorporation method used, Mg is able to improve the performance of the Ni-zeolite catalysts. Magnesium impregnation at lower contents (below 2.5%) over a 5%Ni/zeolite leads to an enhancement of the CO2 conversion into methane of 15% at 350–450 °C, probably due to the induced increase of the Ni particle dispersion, as well as to the possible activation of CO2 on the defects present on the MgO surface. At higher Mg contents, the stronger interaction between Ni and Mg oxides, leading to the formation of NiO–MgO solid solutions, seems to reduce the reducibility of the Ni species, decreasing the amount of nickel active sites available and thus the catalytic performance. Furthermore, important improvements of the catalytic performance (CO2 conversion and CH4 selectivity increased around 20% at 350–450 °C) were also found for the Mg-exchanged 5%Ni/zeolite. The results are comparable to those obtained by impregnation, but lower Mg contents are required. The enhanced activation of CO2 on Mg2+, the more dispersed Ni particles on the support, as well as the enhanced Ni reducibility when compared to the impregnated catalysts can explain the observed results. The beneficial effect of the Mg addition both by impregnation and ion exchange was also observed for samples containing higher amounts of Ni, the best sample remaining stable after 10 h under reaction conditions. Thus, Mg could be an interesting promoter for CO2 methanation over Ni-zeolite catalysts.

AB - CO2 methanation was studied over Ni–Mg–USY zeolite catalysts. Mg was added by incipient wetness impregnation and ion exchange. Whatever the Mg incorporation method used, Mg is able to improve the performance of the Ni-zeolite catalysts. Magnesium impregnation at lower contents (below 2.5%) over a 5%Ni/zeolite leads to an enhancement of the CO2 conversion into methane of 15% at 350–450 °C, probably due to the induced increase of the Ni particle dispersion, as well as to the possible activation of CO2 on the defects present on the MgO surface. At higher Mg contents, the stronger interaction between Ni and Mg oxides, leading to the formation of NiO–MgO solid solutions, seems to reduce the reducibility of the Ni species, decreasing the amount of nickel active sites available and thus the catalytic performance. Furthermore, important improvements of the catalytic performance (CO2 conversion and CH4 selectivity increased around 20% at 350–450 °C) were also found for the Mg-exchanged 5%Ni/zeolite. The results are comparable to those obtained by impregnation, but lower Mg contents are required. The enhanced activation of CO2 on Mg2+, the more dispersed Ni particles on the support, as well as the enhanced Ni reducibility when compared to the impregnated catalysts can explain the observed results. The beneficial effect of the Mg addition both by impregnation and ion exchange was also observed for samples containing higher amounts of Ni, the best sample remaining stable after 10 h under reaction conditions. Thus, Mg could be an interesting promoter for CO2 methanation over Ni-zeolite catalysts.

KW - CO2 methanation

KW - Ni–Mg–USY zeolite catalysts

KW - ion exchange

KW - oxides

KW - catalytic performance

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Bacariza MC, Graça I, Bebiano SS, Lopes JM, Henriques C. Magnesium as promoter of CO2 methanation on Ni-based USY zeolites. Energy and Fuels. 2017 Sep 21;31(9):9776–9789. https://doi.org/10.1021/acs.energyfuels.7b01553