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Highly selective and stable Ni/La-M (M=Sm, Pr, and Mg)-CeO2 catalysts for CO2 methanation

Siakavelas Georgios I., Charisiou Nikolaos, Alkhoori Ayesha, AlKhoori Sara I. , Sebastian Victor, Hinder Steven J., Baker Mark A., Gentekakis Ioannis, Polychronopoulou Kyriaki, Goula Maria A.

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Year 2021
Type of Item Peer-Reviewed Journal Publication
Bibliographic Citation G. I. Siakavelas, N. D. Charisiou, A. AlKhoori, S. AlKhoori, V. Sebastian, S. J. Hinder, M.A.Baker, I. V. Yentekakis, K. Polychronopoulou, and M. A. Goula, “Highly selective and stable Ni/La-M (M=Sm, Pr, and Mg)-CeO2 catalysts for CO2 methanation,” J. CO2 Util., vol. 51, Sep. 2021, doi: 10.1016/j.jcou.2021.101618.
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In the study presented herein, nickel catalysts supported on CeO2 and, for the first time in the literature, on La2O3-Sm2O3-CeO2, La2O3-Pr2O3-CeO2 and La2O3-MgO-CeO2 were prepared and evaluated for the reaction of CO2 methanation. The carriers were prepared through a sol-gel microwave assisted method and the catalysts were obtained following wet impregnation. The physicochemical properties of the catalysts prior to reaction were determined through H2-TPR, H2-TPD, Raman spectroscopy, XRD, CO2-TPD, N2 physisorption-desorption, XPS and TEM. The spent catalysts, after the time-on-stream experiments were further characterised using TEM and TGA. It was shown that the simultaneous incorporation of La3+, Pr3+ and La3+, Sm3+ into the crystal structure of cerium oxide created higher population of oxygen vacant sites. Moreover, the co-presence of La3+, Mg2+ and La3+, Pr3+ into the CeO2 increased the plethos of moderate basic sites. These physicochemical properties increased the rate of CO2 methanation reaction at relatively low temperatures. Furthermore, it is argued that the addition of La3+ stabilized the Ni active sites via the probable formation of a new compound (La-O-Ni) on the catalyst surface or synergetic catalytic centers at the interfacial area improving the catalytic properties (activity and stability). Finally, the catalytic performance tests revealed that the addition of La3+ mainly improved the conversion of CO2 and yield of CH4 for the Ni/La-Mg-Ce and Ni/La-Sm-Ce samples. The rCO2 and XCO2 values at 300 °C followed the order Ni/La-Sm-Ce >> Ni/La-Mg-Ce > Ni/La-Pr-Ce > Ni/Ce.