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

Tsiotsias, Anastasios I.; Charisiou, Nikolaos D.; AlKhoori, Ayesha A.; Gaber, Safa; Stolojan, Vlad; Sebastián, Víctor; Linden, Bart van der; Bansode, Atul; Hinder, Steven J.; Baker, Mark; Polychronopoulou, Kyriaki; Goula, Maria A.

doi:10.1016/j.jechem.2022.04.003

Cited by 52 publications

(45 citation statements)

References 70 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The activation energy of the CO 2 hydrogenation ( E a ) was calculated from the Arrhenius plots, i.e., plots of the natural logarithm of the CO 2 consumption rate as a function of reciprocal temperature. As shown in Figure 1c the E a is around 85 kJ mol −1 , which is among the lowest‐reported for CO 2 methanation over Ni‐based catalysts (typically around 120 kJ mol −1 ) [26, 27] suggesting facile activation of CO 2 over NiCeO x , in line with the high mass‐specific activity.…”

Section: Resultsmentioning

confidence: 62%

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Barreau

Saluso

et al. 2023

Angewandte Chemie

View full text Add to dashboard Cite

CO 2 hydrogenation to methane is gaining increasing interest as one of the most promising ways to store intermittent renewable energy in the form of chemical fuels. Ni particles supported on CeO 2 represent a highly efficient, stable and inexpensive catalyst for this reaction. Herein, Ni-doped CeO 2 nanoparticles were tested for CO 2 methanation showing an extremely high Ni mass-specific activity and CH 4 selectivity. Operando characterization reveals that this performance is tightly associated with ionic Νi and Ce 3 + surface sites, while formation of metallic Ni does not seem to considerably promote the reaction. Theoretical calculations confirmed the stability of interstitial ionic Ni sites on ceria surfaces and highlighted the role of Ce-O frustrated Lewis pair (FLP), Ni-O classical Lewis pair (CLP) and Ni-Ce pair sites to the activation of H 2 and CO 2 molecules. To a large extent, the theoretical predictions were validated by in situ spectroscopy under H 2 and CO 2 : H 2 gaseous environments.

show abstract

Section: Resultsmentioning

confidence: 62%

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Barreau

Saluso

et al. 2023

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

“…Recently, Tsiotsias et al 148 found that an appropriate amount of Pr 3+ cations tended to substitute Ce 4+ ions in the CeO 2 lattice and further induced the generation of oxygen vacancies. On the contrary, a high Pr loading (>20%) decreased the concentration of oxygen vacancies.…”

Section: Strategies To Raise the Catalytic Performance Over Ceria-bas...mentioning

confidence: 99%

Progress in reaction mechanisms and catalyst development of ceria-based catalysts for low-temperature CO₂methanation

Xie

Wen

et al. 2023

Green Chem.

View full text Add to dashboard Cite

show abstract

“…To this end, many noble-metal catalysts (Ru, Rh, and Pd) have been developed; − nevertheless, their scarcity and high price hindered their applications. On the other hand, Ni-based catalysts have gotten more expansive attention in the use of CO 2 methanation because of their outstanding catalytic activity, selectivity, and low cost, and plenty of Ni-based catalysts have been developed, aimed at improving the catalytic performance of the Sabatier reaction. − …”

Section: Introductionmentioning

confidence: 99%

Construction of the Low-Loading Ni/CeO₂ Catalyst with a Boosted CO₂ Methanation Performance via the Facile Pyrolysis CeO₂ Support

Shen

Bai

et al. 2022

Ind. Eng. Chem. Res.

View full text Add to dashboard Cite

Ni-loaded CeO 2 -based materials are one type of the promising catalyst for CO 2 methanation; however, lowering the Ni loading, simplifying the preparation process of CeO 2 supports, and improving the low-temperature catalytic performance are always essential for scalable applications. Herein, an efficient CeO 2 support (CeO 2 -NC) with a large inner pore size was prepared by a facilely controlled calcination of cerium nitrate [Ce(NO 3 ) 3 •6H 2 O] method. On the basis of CeO 2 -NC, one catalyst (Ni/CeO 2 -NC) with low Ni loading (2.56 wt %), desirable Ni dispersity, and abundant medium basic sites was developed that exhibited the amazing low-temperature CO 2 methanation performance. At 275 °C, CO 2 conversion reached up to 77.7% with an almost 100% CH 4 selectivity under a high gas hourly space velocity of 60000 mL g cat −1 h −1 , and the Ni-based mass-specific CH 4 formation rate at 300 °C was up to 4740 μmol g Ni −1 s −1 , outperforming most of the reported Ni-based catalysts to date. The in situ diffuse-reflectance infrared Fourier transform spectroscopy experiments revealed that plentiful active bidentate carbonate intermediates and effective suppression of the dissociated active H species recombination contributed to the boosted CO 2 methanation performance of Ni/CeO 2 -NC at low temperatures. Moreover, the mechanism was also inferred. This work provides new insight into simple pyrolysis CeO 2 supports and should be of significance for the rational design of highly efficient CO 2 methanation catalysts.

show abstract

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

Cited by 52 publications

References 70 publications

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Progress in reaction mechanisms and catalyst development of ceria-based catalysts for low-temperature CO₂methanation

Construction of the Low-Loading Ni/CeO₂ Catalyst with a Boosted CO₂ Methanation Performance via the Facile Pyrolysis CeO₂ Support

Contact Info

Product

Resources

About

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

Cited by 52 publications

References 70 publications

Ionic Nickel Embedded in Ceria with High Specific CO2 Methanation Activity

Ionic Nickel Embedded in Ceria with High Specific CO2 Methanation Activity

Progress in reaction mechanisms and catalyst development of ceria-based catalysts for low-temperature CO2methanation

Construction of the Low-Loading Ni/CeO2 Catalyst with a Boosted CO2 Methanation Performance via the Facile Pyrolysis CeO2 Support

Contact Info

Product

Resources

About

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Ionic Nickel Embedded in Ceria with High Specific CO₂ Methanation Activity

Progress in reaction mechanisms and catalyst development of ceria-based catalysts for low-temperature CO₂methanation

Construction of the Low-Loading Ni/CeO₂ Catalyst with a Boosted CO₂ Methanation Performance via the Facile Pyrolysis CeO₂ Support