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Ni-Based SBA-15 Catalysts Modified with CeMnOx for CO2 Valorization via Dry Reforming of Methane: Effect of Composition on Modulating Activity and H2/CO Ratio Full article

Journal Nanomaterials
, E-ISSN: 2079-4991
Output data Year: 2023, Volume: 13, Number: 19, Article number : 2641, Pages count : 20 DOI: 10.3390/nano13192641
Tags dry reforming of methane (DRM); CeO2–MnOx; Ni-based catalysts; SBA-15; SAXS; Raman spectra
Authors Grabchenko Maria V. 1 , Dorofeeva Natalia V. 1 , Svetlichnyi Valery A. 2 , Larichev Yurii V. 3 , La Parola Valeria 4 , Liotta Leonarda Francesca 4 , Kulinich Sergei A. 5 , Vodyankina O.V. 1
Affiliations
1 Laboratory of Catalytic Research, Tomsk State University, 634050 Tomsk, Russia
2 Laboratory of Advanced Materials and Technology, Siberian Physical Technical Institute, Tomsk State University, 634050 Tomsk, Russia
3 Boreskov Institute of Catalysis SB RAS (BIC SB RAS), 630090 Novosibirsk, Russia
4 Institute for the Study of Nanostructured Materials (ISMN), National Research Council (CNR), 90146 Palermo, Italy
5 Research Institute of Science & Technology, Tokai University, Hiratsuka, Kanagawa 259-1292, Japan

Funding (1)

1 Russian Science Foundation 19-73-30026 (АААА-А19-119052990037-6)

Abstract: Dry reforming of methane with ratio CH4/CO2 = 1 is studied using supported Ni catalysts on SBA-15 modified by CeMnOx mixed oxides with different Ce/Mn ratios (0.25, 1 and 9). The obtained samples are characterized by wide-angle XRD, SAXS, N2 sorption, TPR-H2, TEM, UV–vis and Raman spectroscopies. The SBA-15 modification with CeMnOx decreases the sizes of NiO nanoparticles and enhances the NiO–support interaction. When Ce/Mn = 9, the NiO forms small particles on the surface of large CeO2 particles and/or interacts with CeO2, forming mixed phases. The best catalytic performance (at 650 °C, CH4 and CO2 conversions are 51 and 69%, respectively) is achieved over the Ni/CeMnOx/SBA-15 (9:1) catalyst. The peculiar CeMnOx composition (Ce/Mn = 9) also improves the catalyst stability: In a 24 h stability test, the CH4 conversion decreases by 18 rel.% as compared to a 30 rel.% decrease for unmodified catalyst. The enhanced catalytic stability of Ni/CeMnOx/SBA-15 (9:1) is attributed to the high concentration of reactive peroxo (O−) and superoxo (O2−) species that significantly lower the amount of coke in comparison with Ni-SBA-15 unmodified catalyst (weight loss of 2.7% vs. 42.2%). Ni-SBA-15 modified with equimolar Ce/Mn ratio or Mn excess is less performing. Ni/CeMnOx/SBA-15 (1:4) with the highest content of manganese shows the minimum conversions of reagents in the entire temperature range (X(CO2) = 4–36%, X(CH4) = 8–58%). This finding is possibly attributed to the presence of manganese oxide, which decorates the Ni particles due to its redistribution at the preparation stage.
Cite: Grabchenko M.V. , Dorofeeva N.V. , Svetlichnyi V.A. , Larichev Y.V. , La Parola V. , Liotta L.F. , Kulinich S.A. , Vodyankina O.V.
Ni-Based SBA-15 Catalysts Modified with CeMnOx for CO2 Valorization via Dry Reforming of Methane: Effect of Composition on Modulating Activity and H2/CO Ratio
Nanomaterials. 2023. V.13. N19. 2641 :1-20. DOI: 10.3390/nano13192641 WOS Scopus РИНЦ AN PMID OpenAlex
Dates:
Submitted: Aug 14, 2023
Accepted: Sep 7, 2023
Published online: Sep 26, 2023
Published print: Oct 1, 2023
Identifiers:
Web of science: WOS:001086260300001
Scopus: 2-s2.0-85173795656
Elibrary: 56104612
Chemical Abstracts: 2023:2161852
PMID: 37836282
OpenAlex: W4387056646
Citing:
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OpenAlex 5
Scopus 6
Elibrary 3
Web of science 6
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