Tailoring the Composition of BaxBO3 (B = Fe, Mn) Mixed Oxides as CO or Soot Oxidation Catalysts in Simulated GDI Engine Exhaust Conditions
Abstract
:1. Introduction
2. Results and Discussion
2.1. Chemical, Morphological, and Structural Characterization
2.2. Surface Properties
2.3. Redox Properties
2.4. O2 Release during Temperature-Programmed Desorption in He (O2-TPD)
2.5. Catalytic Activity
3. Materials and Methods
3.1. Synthesis and Characterization of Catalysts
3.2. Activity Tests
4. Conclusions
- (1)
- Manganese-based samples present a BaMnO3 hexagonal perovskite structure, as the decrease in the amount of Ba does not significantly modify the crystalline structure. For iron-based samples, the decrease in the Ba content promotes the transition from a BaFeO2.67 hexagonal perovskite structure to a BaFe2O4 spinel structure.
- (2)
- To compensate for the Ba deficiency in the manganese-based samples, the amount of Mn(IV) and the oxygen vacancies increases, allowing a higher reducibility and oxygen mobility. In iron-based samples, the Ba deficiency only causes a change in the structure from perovskite to spinel.
- (3)
- Manganese-based perovskites (BM-E and B0.7M-E) show a better catalytic performance than iron-based perovskite (BF) for CO oxidation reactions due to the higher generation of actives sites.
- (4)
- The decrease in the Ba content improves the catalytic performance of both catalysts, as B0.7M-E is more active than BM-E for CO oxidation, and B0.7F-E presents a higher activity for soot conversion than BF under simulated GDI engine exhaust conditions. This shows that the composition of BaBO3 mixed oxides can be tailored as function of the oxidation reaction to be catalyzed.
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Catalyst | Average Crystal Size (nm) 1 | |||
---|---|---|---|---|
a | b | c | ||
BM-E | 24.76 | 5.69 | 5.69 | 4.81 |
B0.7M-E | 18.24 | 5.69 | 5.69 | 4.81 |
BF | 49.52 | 5.67 | 5.67 | 13.96 |
B0.7F-E | 23.09 | 19.02 | 5.38 | 8.48 |
Catalyst | BET Surface Area (m2/g) | Chemical Composition (wt %) | |||||
---|---|---|---|---|---|---|---|
Experimental | Nominal | ||||||
Ba | Mn or Fe | O | Ba | Mn or Fe | O | ||
BM-E | 9 | 62 | 24 | 14 | 57 | 23 | 20 |
B0.7M-E | 11 | 55 | 30 | 15 | 48 | 28 | 24 |
BF | 9 | 59 | 24 | 17 | 58 | 24 | 18 |
B0.7F-E | 10 | 51 | 30 | 19 | 44 | 36 | 20 |
Catalyst | Mn(III)/Mn(IV) | Fe(III)/Fe(IV) | XPS OL/(Ba + Mn/Fe) (Nominal) |
---|---|---|---|
BM-E | 5.3 | - | 1.2 (1.5) |
B0.7M-E | 2.1 | - | 1.2 (1.8) |
BF | - | 0.6 | 1.1 (1.5) |
B0.7F-E | - | 0.9 | 1.4 (1.3 1) |
Catalyst | T50% (0.1% CO, 1% O2) (°C) | T50% (1% CO, 1% O2) (°C) | ΔT50% (°C) |
---|---|---|---|
BM-E | 364 | 446 | 82 |
B0.7M-E | 249 | 307 | 58 |
BF | 461 | 352 | −109 |
B0.7F-E | 471 | 437 | −34 |
1% Pt/Al2O3 | 114 | 212 | 98 |
Catalyst | 1% O2/He | 100% He | ||||
---|---|---|---|---|---|---|
T25% (°C) | T50% (°C) | SCO2 (%) | T25% (°C) | T50% (°C) | SCO2 (%) | |
BM-E | 666 | 701 | 67 | 816 | 847 | 8 |
B0.7M-E | 665 | 702 | 78 | 830 | 855 | 11 |
BF | 674 | 710 | 71 | 794 | - | 42 |
B0.7F-E | 653 | 686 | 63 | 892 | - | 33 |
Uncatalyzed | 679 | 718 | 42 | - | - | - |
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Díaz-Verde, Á.; Montilla-Verdú, S.; Torregrosa-Rivero, V.; Illán-Gómez, M.-J. Tailoring the Composition of BaxBO3 (B = Fe, Mn) Mixed Oxides as CO or Soot Oxidation Catalysts in Simulated GDI Engine Exhaust Conditions. Molecules 2023, 28, 3327. https://doi.org/10.3390/molecules28083327
Díaz-Verde Á, Montilla-Verdú S, Torregrosa-Rivero V, Illán-Gómez M-J. Tailoring the Composition of BaxBO3 (B = Fe, Mn) Mixed Oxides as CO or Soot Oxidation Catalysts in Simulated GDI Engine Exhaust Conditions. Molecules. 2023; 28(8):3327. https://doi.org/10.3390/molecules28083327
Chicago/Turabian StyleDíaz-Verde, Álvaro, Salvador Montilla-Verdú, Verónica Torregrosa-Rivero, and María-José Illán-Gómez. 2023. "Tailoring the Composition of BaxBO3 (B = Fe, Mn) Mixed Oxides as CO or Soot Oxidation Catalysts in Simulated GDI Engine Exhaust Conditions" Molecules 28, no. 8: 3327. https://doi.org/10.3390/molecules28083327