Ni-BaMnO3 Perovskite Catalysts for NOx-Assisted Soot Oxidation: Analyzing the Effect of the Nickel Addition Method
Abstract
:1. Introduction
2. Results and Discussion
2.1. BaMn1−xNixO3 Catalysts: Effect of Nickel Content
2.1.1. Chemical and Morphological Properties
2.1.2. Crystalline Structure
2.1.3. Surface Properties
2.1.4. Reducibility
2.1.5. Catalytic Activity Tests
NO to NO2 Oxidation (NOx–TPR)
Soot Oxidation (Soot–NOx–TPR)
2.2. Effect of Nickel Addition Method
2.2.1. Characterization of BMN2H and M5 Catalysts
2.2.2. Catalytic Activity Tests
NO to NO2 Oxidation (NOx–TPR)
Stability Tests
3. Experimental Section
3.1. Synthesis and Characterization of Catalysts
3.2. Activity Tests
4. Conclusions
- -
- Nickel is not incorporated into the lattice of the BaMnO3 perovskite as it forms a BaNiO3 perovskite. If the sol–gel or hydrothermal method is used for nickel addition, an oxygen-deficient perovskite structure (BaNiO2.55) is also detected.
- -
- Mn(III) and Mn(IV) oxidation states coexist on the surface of samples, with Mn(IV) being the main one in most of them. BaMn1−xNixO3 catalysts present oxygen vacancies to compensate for the positive charge imbalance caused by the presence of Mn(III) and Ni(II).
- -
- For nickel samples, a Ni–Mn synergistic effect exists which decreases the manganese reduction temperature during H2–TPR.
- -
- All samples increase the activity for the oxidation of NO and soot at T < 400 °C, with the nickel-containing samples showing the highest activity. BMN2E and BMN4E also present a higher selectivity to CO2 than BME, so it seems that nickel catalysts have more active sites for total soot oxidation. However, no effect of nickel amount in the catalytic performance was observed.
- -
- The method used for nickel addition to BaMnO3 perovskite seems to be relevant as BMN2H, synthetized by hydrothermal procedure, is more active than M5 (obtained by incipient wetness impregnation of BaMnO3) and than BMN2E (obtained by the sol–gel method) as it presents: (i) more surface oxygen vacancies which are active sites for oxidation reactions, (ii) improved redox properties, and (iii) a lower NiO average crystal size which enables a higher amount of nickel active sites for NO and soot oxidation. As a consequence of these properties, BMN2H features a high soot oxidation rate, which minimizes the accumulation of soot and, thus, the deactivation of the catalyst during the reaction.
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
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Sample | Nomenclature | BET Surface Area (m2/g) | Nominal Ni (wt %) | Actual Ni (wt %) | 2θ for Main Peak of BaMnO3 (°) | NiO Average Crystal Size (nm) |
---|---|---|---|---|---|---|
BaMnO3 | BME | 7 | - | - | 31.4 | - |
BaMn0.8Ni0.2O3 | BMN2E | 5 | 4.8 | 4.8 | 31.4 | 30 |
BaMn0.6Ni0.4O3 | BMN4E | 6 | 9.6 | 9.5 | 31.4 | 35 |
Sample | t Factor (Ni2+, Fe3+) |
---|---|
BaMnO3 | 1.09 |
BaMn0.8Ni0.2O3 | 1.07 |
BaMn0.6Ni0.4O3 | 1.06 |
BaNiO3 | 1.02 |
Samples | B.E Max Mn(III) (eV) | B.E Max Mn(VI) (eV) | B.E Max OL (eV) | Ni (wt %) ICP-OES | Ni (wt %) XPS | Surface Ni (%) 1 | NiO/ BaNiO3 2 | Mn(IV)/ Mn(III) | OL/ Mn+Ni+Ba |
---|---|---|---|---|---|---|---|---|---|
BME | 641.3 | 642.4 | 528.9 | - | - | - | - | 1.4 | 0.9 |
BMN2E | 641.8 | 642.8 | 529.4 | 4.8 | 3.5 | 73 | 0.5 | 1.4 | 0.8 |
BMN4E | 641.2 | 642.2 | 529.0 | 9.5 | 8.0 | 84 | 0.7 | 1.3 | 0.7 |
Sample | T50% (°C) | Selectivity to CO2 (%) |
---|---|---|
BME | 563 ± 8 | 75 |
BMN2E | 548 ± 8 | 84 |
BMN4E | 546 ± 8 | 83 |
Blank | 593 ± 8 | 38 |
Sample | 2θ for Main Peak of BaMnO3 (°) | NiO Average Crystal Size (nm) |
---|---|---|
M5 | 31.4 | 24 |
BMN2H | 31.4 | 19 |
Catalyst |
B.E Max
Mn(III) (eV) |
B.E Max
Mn(VI) (eV) |
B.E Max
OL (eV) | Ni (wt %) ICP-OES | Ni (wt %) XPS | Surface Ni (%) 1 | NiO/ BaNiO3 2 | Mn(IV)/ Mn(III) | OL/ Mn+Ni+Ba |
---|---|---|---|---|---|---|---|---|---|
M5 | 641.5 | 643.1 | 529.0 | 4.9 | 20.2 | 412 | 0.7 | 0.6 | 2.0 |
BMN2H | 641.2 | 642.3 | 528.9 | 4.9 | 9.8 | 200 | 0.9 | 0.9 | 1.1 |
Sample | T50% (°C) | Selectivity CO2 (%) |
---|---|---|
M5 | 523 ± 8 | 92 |
BMN2H | 490 ± 8 | 93 |
Blank | 593 ± 8 | 38 |
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Montilla-Verdú, S.; Díaz-Verde, Á.; Torregrosa-Rivero, V.; Illán-Gómez, M.J. Ni-BaMnO3 Perovskite Catalysts for NOx-Assisted Soot Oxidation: Analyzing the Effect of the Nickel Addition Method. Catalysts 2023, 13, 1453. https://doi.org/10.3390/catal13111453
Montilla-Verdú S, Díaz-Verde Á, Torregrosa-Rivero V, Illán-Gómez MJ. Ni-BaMnO3 Perovskite Catalysts for NOx-Assisted Soot Oxidation: Analyzing the Effect of the Nickel Addition Method. Catalysts. 2023; 13(11):1453. https://doi.org/10.3390/catal13111453
Chicago/Turabian StyleMontilla-Verdú, Salvador, Álvaro Díaz-Verde, Verónica Torregrosa-Rivero, and María José Illán-Gómez. 2023. "Ni-BaMnO3 Perovskite Catalysts for NOx-Assisted Soot Oxidation: Analyzing the Effect of the Nickel Addition Method" Catalysts 13, no. 11: 1453. https://doi.org/10.3390/catal13111453