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Peer-reviewedCC BYInternational Journal of Hydrogen Energy

Tailoring Upsalite-derived Ni-MgO catalysts: Impact of synthesis method on CO2 methanation performance

Abstract

CO 2 methanation offers the dual benefits of emission mitigation and energy storage. MgO is considered an ideal support for this process due to its high alkalinity and excellent CO 2 adsorption capacity. In this study, a series of Ni-MgO materials (c.a. 10 wt% Ni) supported on high-surface-area MgO (up to 100 m 2 /g) derived from the thermal treatment of Upsalite® were synthesized using various methods (wet impregnation (WET), incipient wetness impregnation (IWI), and one-pot (OP)) and evaluated for CO 2 methanation. Among them, the catalyst prepared via wet impregnation of mesoporous magnesium carbonate exhibited the highest activity, achieving 86 % CO 2 conversion and 100 % selectivity towards methane at 350 °C. In all cases, the size of the Ni nanoparticles did not increase during the methanation test, even for the longest exposition times, as a result of strong metal–support interactions (SMSI) between Ni and MgO. Ni atom redistribution could be emphasized for Ni-MgO prepared by the IWI and OP methods, leading to smaller particles after the test, but in the end, the best catalyst (WET) was not the one with the smallest Ni nanoparticles but the one showing very constant nanoparticle size throughout methanation. The WET sample was also characterized by the highest percentage of reduced Ni, the highest number of basic sites (CO 2 TPD), and the lowest surface oxygen species (XPS). Furthermore, in situ DRIFTS analyses confirmed that CO 2 methanation over Ni/MgO proceeds via the formate pathway, with HCOO∗ identified as the key intermediate. These results underscore the synergistic effect of Ni nanoparticles and MgO support and provide valuable insights for the rational design of highly efficient Ni-based catalysts for CO 2 methanation. • Ni-MgO solids were synthesized from Upsalite® using 3 approaches. • Ni-MgO from wet impregnation led to the highest activity in methanation. • Strong metal–support interactions ensure abundant active sites and stability. • Ni atoms redistribution was observed for some synthesis approaches. • CO 2 methanation followed the formate pathway (HCOO∗ intermediate).

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BibTeX
@article{sun2026tailoring,
  title = {{Tailoring Upsalite-derived Ni-MgO catalysts: Impact of synthesis method on CO2 methanation performance}},
  author = {Hefei Sun and Neha Choudhary and Jean-Marc Krafft and Patrick Da Costa and Franck Launay},
  journal = {International Journal of Hydrogen Energy},
  year = {2026},
  month = oct,
  doi = {10.1016/j.ijhydene.2025.153173},
  url = {https://hal.science/hal-05791417v1},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Tailoring Upsalite-derived Ni-MgO catalysts: Impact of synthesis method on CO2 methanation performance
AU  - Hefei Sun
AU  - Neha Choudhary
AU  - Jean-Marc Krafft
AU  - Patrick Da Costa
AU  - Franck Launay
PY  - 2026
DA  - 2026/10/10
JO  - International Journal of Hydrogen Energy
DO  - 10.1016/j.ijhydene.2025.153173
UR  - https://hal.science/hal-05791417v1
AB  - CO 2 methanation offers the dual benefits of emission mitigation and energy storage. MgO is considered an ideal support for this process due to its high alkalinity and excellent CO 2 adsorption capacity. In this study, a series of Ni-MgO materials (c.a. 10 wt% Ni) supported on high-surface-area MgO (up to 100 m 2 /g) derived from the thermal treatment of Upsalite® were synthesized using various methods (wet impregnation (WET), incipient wetness impregnation (IWI), and one-pot (OP)) and evaluated for CO 2 methanation. Among them, the catalyst prepared via wet impregnation of mesoporous magnesium carbonate exhibited the highest activity, achieving 86 % CO 2 conversion and 100 % selectivity towards methane at 350 °C. In all cases, the size of the Ni nanoparticles did not increase during the methanation test, even for the longest exposition times, as a result of strong metal–support interactions (SMSI) between Ni and MgO. Ni atom redistribution could be emphasized for Ni-MgO prepared by the IWI and OP methods, leading to smaller particles after the test, but in the end, the best catalyst (WET) was not the one with the smallest Ni nanoparticles but the one showing very constant nanoparticle size throughout methanation. The WET sample was also characterized by the highest percentage of reduced Ni, the highest number of basic sites (CO 2 TPD), and the lowest surface oxygen species (XPS). Furthermore, in situ DRIFTS analyses confirmed that CO 2 methanation over Ni/MgO proceeds via the formate pathway, with HCOO∗ identified as the key intermediate. These results underscore the synergistic effect of Ni nanoparticles and MgO support and provide valuable insights for the rational design of highly efficient Ni-based catalysts for CO 2 methanation. • Ni-MgO solids were synthesized from Upsalite® using 3 approaches. • Ni-MgO from wet impregnation led to the highest activity in methanation. • Strong metal–support interactions ensure abundant active sites and stability. • Ni atoms redistribution was observed for some synthesis approaches. • CO 2 methanation followed the formate pathway (HCOO∗ intermediate).
SN  - 0360-3199
SN  - 1879-3487
ER  -