Advances in Designing Efficient La-Based Perovskites for the NOx Storage and Reduction Process
Abstract
:1. Introduction
2. NO Oxidation over La-Based Perovskites
3. NOx Storage
Catalyst Formulation (Preparation Method) | Reaction Conditions | NOx Storage, μmol g−1 (Temperature, °C) | Ref. |
---|---|---|---|
K2O/LaCoO3/ZrTiO4 (impregnation) | 400 ppm NO/5% O2/N2; GHSV = 60,000 mL g−1 h−1 | 325.0 (350) | [57] |
Pt/La0.5Sr0.5Fe0.5Ti0.5O3/Al2O3 (impregnation) | 500 ppm NO/500 ppm CO/200 ppm C3H6/9% H2O/9% CO2/6.5% O2; GHSV = 80,000 h−1 | 117.0 (250) 150.0 (350) 50.0 (450) | [59] |
La0.7Sr0.3CoO3 (sol-gel) | 400 ppm NO/ 5% O2/ balanced N2; GHSV = 120,000 mL g−1 h−1 | 967.3 (300) | [67] |
LaMn0.9Fe0.1O3 (combustion) | 500 ppm NO/8% O2/N2; GHSV = 30,000 h−1 | 371.6 (100) 392.3 (300) 306.3 (400) | [69] |
LaCoO3 (sol-gel) | 400 ppm NO/5% O2/N2; GHSV = 80,000 mL g−1 h−1 | 93.0 (350) | [73] |
Mesoporous LaCoO3 (nano-casting) | 400 ppm NO/5% O2/N2; GHSV = 80,000 mL g−1 h−1 | 981.0 (350) | [73] |
La0.7Sr0.3CoO3 (sol-gel) | 800 ppm NO/5% O2/ N2; GHSV = 80,000 mL g−1 h−1 | 700.0 (300) | [76] |
La0.7Sr0.3MnO3 (sol-gel) | 800 ppm NO/5% O2/ N2; GHSV = 80,000 mL g−1 h−1 | 170.4 (350) | [77] |
K2O/LaCoO3/(Y,Ce,Zr)O2 (impregnation) | 400 ppm NO/5% O2/N2; GHSV = 45,000 h−1 | 639.0 (350) | [79] |
LaCoO3/3% K2O/CeO2 (impregnation) | 400 ppm NO/5% O2/N2; GHSV = 45,000 h−1 | 512.4 (350) | [80] |
30% Pd/La0.7Sr0.3CoO3/Al2O3 (impregnation) | 500 ppm NO/6% O2/Ar; GHSV = 123,500 h−1 | 97.3 (350) | [83] |
La0.7Sr0.3CoO3/mesoporous SiO2 (deposition) | 500 ppm NO/ 5% O2/ N2; GHSV = 80,000 mL g−1 h−1 | 5269.2 (300) | [84] |
La0.7Sr0.3CoO3 (sol-gel) | 500 ppm NO/5% O2/ N2; GHSV = 80,000 mL g−1 h−1 | 2405.0 (300) | [84] |
4. NOx Desorption and Reduction
Catalyst (Preparation Method) | Reaction Conditions | DeNOx Activity, % (Temperature, °C) | Ref. |
---|---|---|---|
La0.5Sr0.3MnO3 (sol-gel) | Lean (50 s): 400 ppm NO/5% O2/ N2; rich: phase (10 s): 1000 ppm C3H6/N2; GHSV = 120,000 mL g−1 h−1 | 43.2 (350) | [31] |
LaCo0.92Pt0.08O3 (sol-gel) | Lean (120 s): 280 ppm NO/8% O2/8% CO2/N2; rich (30 s): 280 ppm NO/ 8% CO2/3.5% H2/ N2, GHSV = 72,000 h−1 (SO2 treatment: 100 ppm SO2/8% O2/ N2 for 45 min; regeneration: 3.5 vol% H2 at 500 °C for 12 h) | 90.9 (350) 25.5 (350, SO2 treatment) 75.5 (350, regeneration) | [66] |
La0.7Sr0.3CoO3 (sol-gel) | Lean (50 s): 400 ppm NO/5% O2/ N2; rich (10 s): 1000 ppm C3H6/N2; GHSV = 120,000 mL g−1 h−1 | 51.6 (300) | [67] |
La0.7Sr0.3Co0.97Pd0.03O3 (sol-gel) | Lean (50 s): 400 ppm NO/ 5% O2/N2; rich (10 s): 1000 ppm C3H6/N2; GHSV = 120,000 mL g−1 h−1 | 74.4 (300) | [67] |
1.4% Pd/La0.7Sr0.3CoO3 (impregnation) | Lean (50 s): 400 ppm NO/5% O2/N2; rich (10 s): 1000 ppm C3H6/ N2; GHSV = 120,000 mL g−1 h−1 | 90.4 (300) | [67] |
LaMn0.9Fe0.1O3 (sol-gel) | Lean (10 min): 500 ppm NO/8% O2/N2; rich (2 min): 1% H2/ N2; GHSV = 10,000 h−1, plasma assisted | >80% (30–300) | [69] |
LaCoO3 (sol-gel) | Lean (3 min): 500 ppm NO/ 1000 ppm C3H6/6.7% O2/N2; rich (1 min): 500 ppm NO/ 1000 ppm C3H6/ N2; GHSV = 80,000 mL g−1 h−1 | 71.4 (300) | [76] |
1.5% Pd/30% La0.7Sr0.3CoO3/Al2O3 (impregnation) | Lean (150 s): 500 ppm NO/6% O2/Ar; rich (20 s): 512 ppm NO/ 3% H2/ Ar; GHSV = 123,500 mL g−1 h−1 | 86.2% (350) | [82] |
La0.7Sr0.3CoO3 (sol-gel, acid wash) | Lean (3 min): 500 ppm NO/5% O2/ N2; rich (1 min): 500 ppm NO/1000 ppm C3H6/ N2; GHSV = 120,000 mL g−1 h−1 | 55.0% (300) | [91] |
0.3% Pt/LaCoO3/K2O/Al2O3 (impregnation) | Lean (120 s): 500 ppm NO/ 8% O2/ Ar2, rich (120 s): 500 ppm NO/3.5%H2/Ar; GHSV = 72,000 mL g−1 h−1 | 80.0 (300) | [93] |
La0.7Ba0.3Fe0.776Nb0.194Pd0.03O3 (glycine-nitrate method) | Lean (54 s): 512 ppm NO/200 ppm C3H6/10% O2/Ar; rich (6 s): 512 ppm NO/200 ppm C3H6/4% CO/Ar; GHSV = 60,000 mL g−1 h−1 | 47.0 (250) | [97] |
La0.7Sr0.3Co0.97Pd0.03O3 (sol-gel) | Lean (2 min): 0 or 100 ppm SO2/ 500 ppm NO/ 6.7% O2/ N2; rich (1 min); 0 or 100 ppm SO2/ 500 ppm NO/ 1000 ppm C3H6/ N2; GHSV = 32,000 h−1 | 100 (325) 99.2 (325, with SO2) | [98] |
2.1%Pd/La0.7Sr0.3MnO3 (sol-gel) | Lean (50 s): 400 ppm NO/5% O2/ N2; rich: phase (10 s): 1000 ppm C3H6/ N2; GHSV = 120,000 mL g−1 h−1 | 90.1 (350) | [99] |
2.1%Pd/La0.7Sr0.3MnO3 (impregnation) | Lean (50 s): 400 ppm NO/5% O2/N2; rich: phase (10 s): 1000 ppm C3H6/N2; GHSV = 120,000 mL g−1 h−1 | 72.0 (350) | [99] |
5. Resistance to Poisoners
6. Conclusions and Perspective
- (1)
- In-depth understanding of the NSR reaction mechanism in perovskites. To date, most mechanism studies concerning the NSR reaction were conducted with a Pt-based model catalyst, while for other types of catalysts, including perovskites, only vague pathways and plausible lines have been proposed. Considering the complexity of the reaction process, more in-depth experimental and theoretical studies should be conducted to unravel the detailed reaction routes, active sites, and intermediates to support the rational design of perovskite formulations with predictable properties.
- (2)
- Comprehensive comparison of NSR performance of La-based perovskites with others. The majority of perovskite-based materials reported for NSR applications over the last decade have been La-based. The obtained data reveals that La3+ provides prominent structural integrity with few impurities and little phase segregation, as well as thermal and chemical stability resistant to phase transformation during NOx storage and reduction. Furthermore, the extensively studied LaCoO3 and LaMnO3 catalytic systems exhibit a good redox property, which is desirable for the NSR reaction. However, the weak basicity of A-site La3+ brings challenges for high-temperature NOx storage, and the usage of La and Co increases environmental burdens from the perspective of sustainability. Some interesting data have been recently reported for Sr- and Ba-based perovskite formulations. On one hand, the stronger basicity of A-site alkaline earth metal provides better high-temperature NOx storage performance, and the +2 oxidation state of the A-site cation increases the B-site oxidation state and/or generates oxygen vacancies desirable for NO oxidation and NOx storage. On the other hand, these strongly basic cations are generally less resistant to CO2, NOx, and SO2 in the reaction atmosphere, and hence are prone to exsolution from the perovskite matrix, leading to the risk of collapse of the perovskite structure, but this tendency may vary depending on specific formulations. At this stage, a comprehensive study of the effects of different A-site cations on the activity and stability of perovskite catalysts in NSR reactions will be rather helpful.
- (3)
- Synergetic/competitive relation between different storage sites. As stated earlier, a practical NSR catalyst should be capable of efficiently trapping and releasing NOx in a wide range of temperatures. This indicates that multiple storage components with different basicity should be used in combination; however, almost no comprehensive research has been devoted to this line. Current research suggests that La-based perovskite is an excellent low-temperature NOx storage component, but whether the combination of perovskite and stronger basic sites efficient for high-temperature NSR reaction can work as they are intended remains unclear.
- (4)
- Redox stability and resistance to H2O, CO2, and SO2 poisoning. Most perovskite formulations are designed and tested under ideal laboratory conditions. The durability of perovskite catalysts in reducing atmosphere or when exposed to the common poisoners in automotive exhaust should be carefully considered and further clarified.
- (5)
- Sustainability has become an essential concern in catalyst design with the guidance of legislation and increasing environmental awareness of the community. However, this is entirely neglected in the currently reviewed publications. The environmental burden of using Pt on a per kilogram basis is calculated to be 3–4 orders of magnitude larger than base metals, in the aspects of global warming potential, cumulative energy demand, terrestrial acidification, freshwater eutrophication, and human toxicity [104], which necessitates the development of environmentally friendly base metal alternatives. Along this line, in perovskite formulation design, the metals at the lower end of the scale of environmental impacts should be preferably considered, such as manganese, iron, and titanium at B-site. These metals also result in decent NSR performance, while the usage of nickel and cobalt should be more prudent. For A-site cations, Sr and Ba are better choices than La.
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Zhao, D.; Song, H.; Liu, J.; Jiang, Q.; Li, X. Advances in Designing Efficient La-Based Perovskites for the NOx Storage and Reduction Process. Catalysts 2022, 12, 593. https://doi.org/10.3390/catal12060593
Zhao D, Song H, Liu J, Jiang Q, Li X. Advances in Designing Efficient La-Based Perovskites for the NOx Storage and Reduction Process. Catalysts. 2022; 12(6):593. https://doi.org/10.3390/catal12060593
Chicago/Turabian StyleZhao, Dongyue, Haitao Song, Jun Liu, Qiuqiao Jiang, and Xingang Li. 2022. "Advances in Designing Efficient La-Based Perovskites for the NOx Storage and Reduction Process" Catalysts 12, no. 6: 593. https://doi.org/10.3390/catal12060593