Balancing performance and sustainability in integrated CO₂ capture and methanation via NiCeO₂-anionic clay hybrid materials
Abstract
Integrated CO₂ capture and methanation (ICCM) provides a direct route for converting captured CO₂ into synthetic methane, but its large-scale implementation is limited by material stability and sustainability. Here, we report NiCeO₂/ionic clay hybrid materials, where the Mg-Al oxide derived from the layered double hydroxide (LDH) clay acts as an adsorbent matrix for NiCeO₂ catalytic nanoparticles. The hybrids exhibit enhanced CO₂ uptake, efficient low-temperature operation (300 °C) with 100% CH₄ selectivity, and excellent cyclic stability under ICCM conditions. Although the NiCeO₂/LDH hybrids show lower methane productivity per unit mass of total material than NiCeO₂ alone, they significantly improve catalyst utilization, producing up to seven times more CH₄ per unit mass of NiCeO₂. Operando XANES reveals a reversible Ni2+/Ni0 redox transition under alternating CO₂/H₂ atmospheres, demonstrating that the active Ni phase dynamically adjusts its oxidation state during CO₂ adsorption–hydrogenation cycles. Life cycle assessment demonstrates a markedly reduced environmental footprint for the hybrid materials compared with NiCeO₂ for the same methane output, highlighting NiCeO₂/LDH hybrids as sustainable and scalable platforms for integrated CO₂ capture and conversion
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BibTeX
@article{morfin2026balancing,
title = {{Balancing performance and sustainability in integrated CO₂ capture and methanation via NiCeO₂-anionic clay hybrid materials}},
author = {F. Morfin and Javier Ivanez and Ruben Checa and L. Piccolo and Anastasia Pappa and F. Zhou and Thierry Dintzer and Mathias Barreau and Haroon Osman Sumbhaniya and Samar Garreau-Hajjar and Liva Dzene and Davide Salusso and Spiros Papaefthimiou and Spiridon Zafeiratos},
journal = {Chemical Engineering Journal},
year = {2026},
month = oct,
doi = {10.1016/j.cej.2026.179101},
url = {https://hal.science/hal-05694620v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Balancing performance and sustainability in integrated CO₂ capture and methanation via NiCeO₂-anionic clay hybrid materials
AU - F. Morfin
AU - Javier Ivanez
AU - Ruben Checa
AU - L. Piccolo
AU - Anastasia Pappa
AU - F. Zhou
AU - Thierry Dintzer
AU - Mathias Barreau
AU - Haroon Osman Sumbhaniya
AU - Samar Garreau-Hajjar
AU - Liva Dzene
AU - Davide Salusso
AU - Spiros Papaefthimiou
AU - Spiridon Zafeiratos
PY - 2026
DA - 2026/10/13
JO - Chemical Engineering Journal
DO - 10.1016/j.cej.2026.179101
UR - https://hal.science/hal-05694620v1
AB - Integrated CO₂ capture and methanation (ICCM) provides a direct route for converting captured CO₂ into synthetic methane, but its large-scale implementation is limited by material stability and sustainability. Here, we report NiCeO₂/ionic clay hybrid materials, where the Mg-Al oxide derived from the layered double hydroxide (LDH) clay acts as an adsorbent matrix for NiCeO₂ catalytic nanoparticles. The hybrids exhibit enhanced CO₂ uptake, efficient low-temperature operation (300 °C) with 100% CH₄ selectivity, and excellent cyclic stability under ICCM conditions. Although the NiCeO₂/LDH hybrids show lower methane productivity per unit mass of total material than NiCeO₂ alone, they significantly improve catalyst utilization, producing up to seven times more CH₄ per unit mass of NiCeO₂. Operando XANES reveals a reversible Ni2+/Ni0 redox transition under alternating CO₂/H₂ atmospheres, demonstrating that the active Ni phase dynamically adjusts its oxidation state during CO₂ adsorption–hydrogenation cycles. Life cycle assessment demonstrates a markedly reduced environmental footprint for the hybrid materials compared with NiCeO₂ for the same methane output, highlighting NiCeO₂/LDH hybrids as sustainable and scalable platforms for integrated CO₂ capture and conversion
SN - 1385-8947
ER -