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. 2021 Sep 27;11(50):31807-31816.
doi: 10.1039/d1ra04115k. eCollection 2021 Sep 21.

Barium promoted Ni/Sm2O3 catalysts for enhanced CO2 methanation

Nur Athirah Ayub  1 , Hasliza Bahruji  1 , Abdul Hanif Mahadi  1
Affiliations

Barium promoted Ni/Sm2O3 catalysts for enhanced CO2 methanation

Nur Athirah Ayub et al. RSC Adv. .

Abstract

Low temperature CO2 methanation is a favorable pathway to achieve high selectivity to methane while increasing the stability of the catalysts. A Ba promoted Ni/Sm2O3 catalyst was investigated for CO2 methanation at atmospheric pressure with the temperature ranging from 200-450 °C. 5Ni-5Ba/Sm2O3 showed significant enhancement of CO2 conversion particularly at temperatures ≤ 300 °C compared to Ni/Sm2O3. Incorporation of Ba into 5Ni/Sm2O3 improved the basicity of the catalysts and transformed the morphology of Sm2O3 from random structure into uniform groundnut shape nanoparticles. The uniformity of Sm2O3 created interparticle porosity that may be responsible for efficient heat transfer during a long catalytic reaction. Ba is also postulated to catalyze oxygen vacancy formation on Sm2O3 under a reducing environment presumably via isomorphic substitution. The disappearance of a high temperature (∼600 °C) reduction peak in H2-TPR analysis revealed the reducibility of NiO following impregnation with Ba. However, further increasing the Ba loading to 15% formed BaNiO3-BaNiO2.36 phases which consequently reduced the activity of the Ni-Ba/Sm2O3 catalyst at low temperature. Ni was suggested to segregate from BaNiO3-BaNiO2.36 at high temperature thus exhibiting comparable activity with Ni/Sm2O3 at 450 °C.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. (a) Wide and (b) narrow angle XRD patterns of pure Sm2O3, 5Ni/Sm2O3 and 5Ni–xBa on Sm2O3 with different Ba loading after calcination at 500 °C.
Fig. 2
Fig. 2. (a) Nitrogen adsorption–desorption isotherms and (b) pore size distribution of 5Ni/Sm2O3 and 5Ni–xBa/Sm2O3,x = 5%, 10% and 15% after calcination at 500 °C.
Fig. 3
Fig. 3. FESEM images of 5Ni–xBa/Sm2O3 at (a) 0% Ba, (b) 5% Ba, (c) 15% Ba and (d) EDX mapping of 5Ni–xBa/Sm2O3 at 5% Ba after calcination.
Fig. 4
Fig. 4. HRTEM analysis of 5Ni–5Ba/Sm2O3 (a and b) and 5Ni–15Ba/Sm2O3 (c and d) after calcination in air at 500 °C.
Fig. 5
Fig. 5. H2-TPR profiles of 5Ni/Sm2O3, 5Ba/Sm2O3, BaO, and 5Ni–xBa/Sm2O3 at different Ba loading. The catalysts were calcined in air at 500 °C prior to the analysis.
Fig. 6
Fig. 6. CO2-TPD profiles of 5Ni/Sm2O3, 5Ba/Sm2O3 and 5Ni–xBa/Sm2O3 with different Ba loading at x = 5%, 10%, 15%.
Fig. 7
Fig. 7. Ni 2p, Sm 3d, O 1s and Ba 3d XPS spectra of 5Ni/Sm2O3 and 5Ni–5Ba/Sm2O3 after reduction at 450 °C.
Fig. 8
Fig. 8. CO2 conversion for 5Ni/Sm2O3 and 5Ni–xBa/Sm2O3 at x = 5%, 10%, 15%. The catalysts was pre-reduced in situ under H2 for 3 h at 450 °C.
Fig. 9
Fig. 9. Catalytic stability of 5Ni–5Ba/Sm2O3 catalysts at 300 °C for 28 h.
Fig. 10
Fig. 10. CO2 conversion and selectivity of 5Ni/Sm2O3 and 5Ni–5Ba/Sm2O3 at different reduction temperature.
See this image and copyright information in PMC

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