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4-ZhaoDebeckerJEnvChemEng2025-C3N4NickelCeO2CO2methanation-preprint.pdf
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Abstract
Selective CO2 methanation using green H2 offers a promising approach for tackling both energy and environmental challenges. Herein, a Ni/CeO2 catalyst was synthesized using a one-pot method in the presence of sacrificial C3N4 and evaluated for CO₂ methanation. The catalyst exhibited a high CO2 conversion of 82.6 % and a CH4 production rate of up to 178 mmol gcat−1 h−1, with high CH4 selectivity (99.4 %) at a remarkably low temperature of 250 °C. Surface characterization techniques, including Raman spectroscopy, XPS, 31P-MAS NMR of adsorbed trimethylphosphine, and CO2-TPD, demonstrate that the addition of C3N4 significantly enhanced the concentration of surface oxygen vacancies and medium-strength basic sites. In situ DRIFTS analysis indicated that CO2 methanation over Ni/CeO2 proceeded via the RWGS+CO hydrogenation and formate pathways, with the former being predominant at low temperatures. The exceptional low-temperature methanation performance of this new catalyst is attributed to the increased density of oxygen vacancies and medium-strength basic sites.
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Zhao, Y., Hongmanorom, P., Yang, F., Casale, S., Sassoye, C., Styskalik, A., & Debecker, D. (2025). Carbon nitride boosts the CO2 methanation activity of Ni/CeO2. Journal of Environmental Chemical Engineering, 13(6), 119153. https://doi.org/10.1016/j.jece.2025.119153 (Original work published 2025)