New Insight into the Interplay of Method of Deposition, Chemical State of Pd, Oxygen Storage Capability and Catalytic Activity of Pd-Containing Perovskite Catalysts for Combustion of Methane
Abstract
:1. Introduction
2. Results and Discussions
2.1. Structure and Texture of Pd-Containing Perovskite Supported on SiO2-Modified/γ-Alumina
2.2. Catalytic Activity of Supported Pd-Containing Perovskite over SiO2-Modified Alumina
2.2.1. Pre-Treatment Tests
2.2.2. Reaction Kinetics
2.3. Ex-Situ XPS Analysis
2.4. Preliminary Data on Possible Practical Application
3. Experimental
3.1. Catalyst Preparation
3.2. Catalyst Characterization
3.3. Catalytic Activity Measurements
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Samples | Signal 1 | Signal 2 | IHE/ILE | ||
---|---|---|---|---|---|
Pd 3d5/2, eV | Line Width, eV | Pd 3d5/2, eV | Line Width, eV | ||
Pd-LMO/Imp—fresh | 336.4 | 1.40 | 337.5 | 2.43 | 0.76 |
Pd-LMO/Imp—after catalytic test | 336.3 | 1.28 | 338.1 | 2.5 | 0.36 |
Pd-LMO/U-AACVD—fresh | 335.9 | 1.45 | 337.2 | 2.2 | 1.67 |
Pd-LMO/U-AACVD—after catalytic test | 336.3 | 1.69 | - | - | 0 |
Sample | S, m2/g | Vt, cm3/g | D, nm |
---|---|---|---|
γ-Al2O3 | 219 | 0.41 | 7.4 |
SiO2 modified γ-Al2O3 | 204 | 0.39 | 7.8 |
Pd-LMO/U-AACVD | 181 | 0.37 | 8.1 |
Pd-LMO/Imp | 172 | 0.36 | 8.7 |
LMO/U-AACVD | 164 | 0.38 | 9.2 |
LMO/Imp | 153 | 0.35 | 9.1 |
Fresh Catalyst | After Working Cycle | |||
---|---|---|---|---|
Reacted Oxygen (Uptake) | mg O2 to CO | mg O2 to CO2 | mg O2 to CO | mg O2 to CO2 |
Pd-LMO/U-AACVD | 1.0 | 0.4 | 2.7 | 0.7 |
Pd-LMO/Imp | 2.6 | 0.8 | 2.3 | 1.0 |
Model: PWL | Catalyst | ko | Ea | m (CH4) | n (O2) | p (H2O) | RSS | R2 |
---|---|---|---|---|---|---|---|---|
Pd-LMO/U-AACVD | 68.3 | 1.36 × 102 | 0.84 | 0.18 | −0.10 | 5.4 | 0.977 | |
Pd-LMO/Imp | 69.2 | 4.14 × 102 | 0.90 | 0.21 | −0.11 | 4.0 | 0.986 |
Model: MVK-1 | Catalyst | ko,ox | Ea,ox | ko,red | Ea,red | ko,water | −ΔHwater | RSS | R2 |
---|---|---|---|---|---|---|---|---|---|
water adsorbs on oxidized sites | Pd-LMO/U-AACVD | 1.29 × 104 | 85.2 | 1.13 × 102 | 56.5 | 4.02 × 103 | 58.0 | 2.7 | 0.988 |
= 2 | Pd-LMO/Imp | 2.90 × 104 | 91.2 | 2.18 × 102 | 56.5 | 6.60 × 103 | 54.4 | 3.4 | 0.980 |
Model: MVK-2 | |||||||||
water adsorbs on reduced sites | Pd-LMO/U-AACVD | 8.39 × 102 | 16.2 | 3.16 × 102 | 62.3 | 5.84 ×1 03 | 82.0 | 4.4 | 0.980 |
= 2 | Pd-LMO/Imp | 2.95 × 102 | 15.3 | 1.99 × 103 | 68.4 | 6.61 × 103 | 72.8 | 4.8 | 0.983 |
Model | Catalyst | ko | Ea | ko,ox | −ΔHox | ko,water | −ΔHwater | RSS | R2 |
---|---|---|---|---|---|---|---|---|---|
ER | Pd-LMO/U-AACVD | 7.42 × 102 | 65.9 | 6.32 × 103 | 65.5 | 2.17 × 103 | 88.4 | 5.2 | 0.971 |
Pd-LMO/Imp | 1.22 × 104 | 76.9 | 9.15 × 105 | 78.0 | 6.39 × 103 | 72.5 | 5.5 | 0.978 |
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Stanchovska, S.; Ivanov, G.; Harizanova, S.; Tenchev, K.; Zhecheva, E.; Naydenov, A.; Stoyanova, R. New Insight into the Interplay of Method of Deposition, Chemical State of Pd, Oxygen Storage Capability and Catalytic Activity of Pd-Containing Perovskite Catalysts for Combustion of Methane. Catalysts 2021, 11, 1399. https://doi.org/10.3390/catal11111399
Stanchovska S, Ivanov G, Harizanova S, Tenchev K, Zhecheva E, Naydenov A, Stoyanova R. New Insight into the Interplay of Method of Deposition, Chemical State of Pd, Oxygen Storage Capability and Catalytic Activity of Pd-Containing Perovskite Catalysts for Combustion of Methane. Catalysts. 2021; 11(11):1399. https://doi.org/10.3390/catal11111399
Chicago/Turabian StyleStanchovska, Silva, Georgy Ivanov, Sonya Harizanova, Krasimir Tenchev, Ekaterina Zhecheva, Anton Naydenov, and Radostina Stoyanova. 2021. "New Insight into the Interplay of Method of Deposition, Chemical State of Pd, Oxygen Storage Capability and Catalytic Activity of Pd-Containing Perovskite Catalysts for Combustion of Methane" Catalysts 11, no. 11: 1399. https://doi.org/10.3390/catal11111399