Optimizing the oxide support composition in Pr-doped CeO2 towards highly active and selective Ni-based CO2 methanation catalysts

Anastasios I. Tsiotsias; Nikolaos D. Charisiou; Ayesha AlKhoori; Safa Gaber; Vlad Stolojan; Victor Sebastian; Bart van der Linden; Atul Bansode; Steven J. Hinder; null More Authors

doi:10.1016/j.jechem.2022.04.003

Optimizing the oxide support composition in Pr-doped CeO₂ towards highly active and selective Ni-based CO₂ methanation catalysts

Anastasios I. Tsiotsias, Nikolaos D. Charisiou, Ayesha AlKhoori, Safa Gaber, Vlad Stolojan, Victor Sebastian, Bart van der Linden, Atul Bansode, Steven J. Hinder, More Authors

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

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Abstract

In this study, Ni catalysts supported on Pr-doped CeO₂ are studied for the CO₂ methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated. It is shown, that Pr³⁺ ions can substitute Ce⁴⁺ ones in the support lattice, thereby introducing a high population of oxygen vacancies, which act as active sites for CO₂ chemisorption. Pr doping can also act to reduce the crystallite size of metallic Ni, thus promoting the active metal dispersion. Catalytic performance evaluation evidences the promoting effect of low Pr loadings (5 at% and 10 at%) towards a higher catalytic activity and lower CO₂ activation energy. On the other hand, higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population, thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.

Original language	English
Pages (from-to)	547-561
Number of pages	15
Journal	Journal of Energy Chemistry
Volume	71
DOIs	https://doi.org/10.1016/j.jechem.2022.04.003
Publication status	Published - 2022

Bibliographical note

Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care
Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

Keywords

Activation energy
Catalytic activity
CO methanation
Ni-based catalyst
Oxygen vacancy
Power-to-gas
Pr-doped CeO

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10.1016/j.jechem.2022.04.003

1-s2.0-S2095495622001930-mainFinal published version, 4.67 MB

Cite this

Tsiotsias, A. I., Charisiou, N. D., AlKhoori, A., Gaber, S., Stolojan, V., Sebastian, V., van der Linden, B., Bansode, A., Hinder, S. J., & More Authors (2022). Optimizing the oxide support composition in Pr-doped CeO₂ towards highly active and selective Ni-based CO₂ methanation catalysts. Journal of Energy Chemistry, 71, 547-561. https://doi.org/10.1016/j.jechem.2022.04.003

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title = "Optimizing the oxide support composition in Pr-doped CeO2 towards highly active and selective Ni-based CO2 methanation catalysts",

abstract = "In this study, Ni catalysts supported on Pr-doped CeO2 are studied for the CO2 methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated. It is shown, that Pr3+ ions can substitute Ce4+ ones in the support lattice, thereby introducing a high population of oxygen vacancies, which act as active sites for CO2 chemisorption. Pr doping can also act to reduce the crystallite size of metallic Ni, thus promoting the active metal dispersion. Catalytic performance evaluation evidences the promoting effect of low Pr loadings (5 at% and 10 at%) towards a higher catalytic activity and lower CO2 activation energy. On the other hand, higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population, thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.",

keywords = "Activation energy, Catalytic activity, CO methanation, Ni-based catalyst, Oxygen vacancy, Power-to-gas, Pr-doped CeO",

author = "Tsiotsias, {Anastasios I.} and Charisiou, {Nikolaos D.} and Ayesha AlKhoori and Safa Gaber and Vlad Stolojan and Victor Sebastian and {van der Linden}, Bart and Atul Bansode and Hinder, {Steven J.} and {More Authors}",

note = "Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.",

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doi = "10.1016/j.jechem.2022.04.003",

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Tsiotsias, AI, Charisiou, ND, AlKhoori, A, Gaber, S, Stolojan, V, Sebastian, V, van der Linden, B , Bansode, A, Hinder, SJ & More Authors 2022, 'Optimizing the oxide support composition in Pr-doped CeO₂ towards highly active and selective Ni-based CO₂ methanation catalysts', Journal of Energy Chemistry, vol. 71, pp. 547-561. https://doi.org/10.1016/j.jechem.2022.04.003

TY - JOUR

T1 - Optimizing the oxide support composition in Pr-doped CeO2 towards highly active and selective Ni-based CO2 methanation catalysts

AU - Tsiotsias, Anastasios I.

AU - Charisiou, Nikolaos D.

AU - AlKhoori, Ayesha

AU - Gaber, Safa

AU - Stolojan, Vlad

AU - Sebastian, Victor

AU - van der Linden, Bart

AU - Bansode, Atul

AU - Hinder, Steven J.

AU - More Authors, null

N1 - Green Open Access added to TU Delft Institutional Repository 'You share, we take care!' - Taverne project https://www.openaccess.nl/en/you-share-we-take-care Otherwise as indicated in the copyright section: the publisher is the copyright holder of this work and the author uses the Dutch legislation to make this work public.

PY - 2022

Y1 - 2022

N2 - In this study, Ni catalysts supported on Pr-doped CeO2 are studied for the CO2 methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated. It is shown, that Pr3+ ions can substitute Ce4+ ones in the support lattice, thereby introducing a high population of oxygen vacancies, which act as active sites for CO2 chemisorption. Pr doping can also act to reduce the crystallite size of metallic Ni, thus promoting the active metal dispersion. Catalytic performance evaluation evidences the promoting effect of low Pr loadings (5 at% and 10 at%) towards a higher catalytic activity and lower CO2 activation energy. On the other hand, higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population, thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.

AB - In this study, Ni catalysts supported on Pr-doped CeO2 are studied for the CO2 methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated. It is shown, that Pr3+ ions can substitute Ce4+ ones in the support lattice, thereby introducing a high population of oxygen vacancies, which act as active sites for CO2 chemisorption. Pr doping can also act to reduce the crystallite size of metallic Ni, thus promoting the active metal dispersion. Catalytic performance evaluation evidences the promoting effect of low Pr loadings (5 at% and 10 at%) towards a higher catalytic activity and lower CO2 activation energy. On the other hand, higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population, thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.

KW - Activation energy

KW - Catalytic activity

KW - CO methanation

KW - Ni-based catalyst

KW - Oxygen vacancy

KW - Power-to-gas

KW - Pr-doped CeO

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