Quality or Quantity? How Structural Parameters Affect Catalytic Activity of Iron Oxides for CO Oxidation
Abstract
:1. Introduction
2. Results
2.1. Structural Characterization
2.2. Catalytic Activity
3. Summary and Conclusions
4. Experimental Methodology
4.1. Preparation of γ-Al2O3
4.2. Preparation of Catalysts Fe01 to Fe20
4.3. Catalytic Experiments
4.4. Analytics
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Sample | BET Surface [m2/g] |
---|---|
γ-Al2O3 | 169 |
Fe01 | 155 |
Fe025 | 164 |
Fe05 | 167 |
Fe10 | 152 |
Fe20 | 121 |
Refined Value | Fe05 | Fe10 | Fe20 |
---|---|---|---|
a(γ-Al2O3) [Å] | 7.935 | 7.949 | 7.962 |
a(γ-Fe2O3) [Å] | 8.025 | 8.062 | 8.327 |
Spherical particle size (Fe2O3) [nm] | 2.2 | 2.9 | 8.5 |
Sample | δ [mm/s] | ΔEQ [mm/s] | Γ [mm/s] | Bhf [T] | |
---|---|---|---|---|---|
Fe01 | 0.26 | 0.90 | 0.80 | ||
Fe025 | 0.29 | 1.01 | 0.70 | ||
Fe05 | 0.28 | 0.96 | 0.70 | ||
Fe10 | doublet | 0.28 | 0.92 | 0.66 | |
sextet | 0.28 | 0 | 0.74/0.69/1.0 | 49.3 | |
Fe20 | doublet | 0.27 | 0.90 | 0.61 | |
sextet | 0.35 | 0 | 0.79/0.78/1.0 | 49.5 |
Catalyst | Fetet [%] | Feoct [%] | FexOy Olig. [%] | FexOy Particles [%] |
---|---|---|---|---|
Fe01 | 12.0 | 37.3 | 50.3 | 0.44 |
Fe025 | 10.8 | 35.4 | 48.6 | 5.15 |
Fe05 | 7.30 | 22.7 | 60.5 | 9.52 |
Fe10 | 4.87 | 17.6 | 57.7 | 19.8 |
Fe20 | 4.20 | 15.2 | 65.7 | 14.9 |
Catalyst | Abs-Bs | N (Bs) | R (Abs-Bs) [Å] | σ [Å−1] | |
---|---|---|---|---|---|
Fe01 | Fe–O | 4.8 ± 0.24 | 1.944 ± 0.019 | 0.089 ± 0.008 | R = 28.29% |
Fe–O | 1.1 ± 0.05 | 2.157 ± 0.021 | 0.045 ± 0.004 | Ef = 3.655 eV | |
Fe–Fe | 1.0 ± 0.10 | 3.059 ± 0.030 | 0.112 ± 0.011 | Afac = 0.9477 | |
Fe–Al | 8.1 ± 0.81 | 3.426 ± 0.034 | 0.112 ± 0.011 | ||
Fe–Fe | 5.0 ± 0.50 | 3.439 ± 0.034 | 0.112 ± 0.011 | ||
Fe025 | Fe–O | 4.6 ± 0.23 | 1.944 ± 0.019 | 0.095 ± 0.009 | R = 38.80% |
Fe–O | 1.6 ± 0.08 | 2.169 ± 0.021 | 0.087 ± 0.008 | Ef = 3.137 eV | |
Fe–Fe | 1.1 ± 0.11 | 3.047 ± 0.030 | 0.107 ± 0.010 | Afac = 0.9072 | |
Fe–Al | 7.9 ± 0.79 | 3.455 ± 0.034 | 0.112 ± 0.011 | ||
Fe–Fe | 5.6 ± 0.56 | 3.463 ± 0.034 | 0.112 ± 0.011 | ||
Fe05 | Fe–O | 3.6 ± 0.18 | 1.911 ± 0.019 | 0.087 ± 0.008 | R = 34.13% |
Fe–O | 3.1 ± 0.15 | 2.076 ± 0.020 | 0.112 ± 0.011 | Ef = 4.013 eV | |
Fe–Fe | 0.8 ± 0.08 | 3.063 ± 0.030 | 0.105 ± 0.010 | Afac = 0.8896 | |
Fe–Al | 7.4 ± 0.74 | 3.397 ± 0.033 | 0.112 ± 0.011 | ||
Fe–Fe | 4.7 ± 0.47 | 3.414 ± 0.034 | 0.112 ± 0.011 | ||
Fe10 | Fe–O | 3.4 ± 0.17 | 1.907 ± 0.019 | 0.081 ± 0.008 | R = 33.88% |
Fe–O | 3.0 ± 0.15 | 2.065 ± 0.020 | 0.112 ± 0.011 | Ef = 2.925 eV | |
Fe–Fe | 0.5 ± 0.05 | 2.983 ± 0.029 | 0.092 ± 0.009 | Afac = 0.8896 | |
Fe–Al | 6.2 ± 0.62 | 3.354 ± 0.033 | 0.112 ± 0.011 | ||
Fe–Fe | 4.0 ± 0.40 | 3.403 ± 0.034 | 0.112 ± 0.011 | ||
Fe20 | Fe–O | 2.5 ± 0.12 | 1.898 ± 0.018 | 0.077 ± 0.007 | R = 33.35% |
Fe–O | 3.9 ± 0.19 | 2.025 ± 0.020 | 0.110 ± 0.011 | Ef = 4.384 eV | |
Fe–Fe | 0.5 ± 0.05 | 2.962 ± 0.029 | 0.081 ± 0.008 | Afac = 0.8217 | |
Fe–Al | 9.0 ± 0.90 | 3.360 ± 0.033 | 0.112 ± 0.011 | ||
Fe–Fe | 5.7 ± 0.57 | 3.394 ± 0.033 | 0.112 ± 0.011 | ||
α-Fe2O3 | Fe–O | 3.2 ± 0.16 | 1.961 ± 0.019 | 0.081 ± 0.008 | R = 27.77% |
Fe–O | 3.3 ± 0.16 | 2.134 ± 0.021 | 0.110 ± 0.011 | Ef = 2.584 eV | |
Fe–Fe | 6.3 ± 0.31 | 2.983 ± 0.029 | 0.112 ± 0.011 | Afac = 0.9735 | |
Fe–Fe | 2.9 ± 0.29 | 3.317 ± 0.033 | 0.112 ± 0.011 | ||
Fe–Fe | 1.2 ± 0.12 | 3.706 ± 0.037 | 0.063 ± 0.006 | ||
γ-Fe2O3 | Fe–O | 0.7 ± 0.03 | 1.868 ± 0.018 | 0.032 ± 0.003 | R = 24.68% |
Fe–O | 4.8 ± 0.14 | 2.003 ± 0.020 | 0.105 ± 0.010 | Ef = 3.112 eV | |
Fe–Fe | 4.4 ± 0.44 | 3.019 ± 0.030 | 0.112 ± 0.011 | Afac = 0.8219 | |
Fe–Fe | 2.1 ± 0.21 | 3.467 ± 0.034 | 0.087 ± 0.008 | ||
Fe–Fe | 3.6 ± 0.36 | 5.128 ± 0.051 | 0.112 ± 0.011 |
Catalyst | TLight-off [°C] (10%) | T30 [°C] | T50 [°C] | T90 [°C] | T95 [°C] |
---|---|---|---|---|---|
Fe01 | 170 | 267 | 362 | 449 | 467 |
Fe025 | 109 | 169 | 211 | 307 | 332 |
Fe05 | 86 | 136 | 169 | 240 | 259 |
Fe10 | 88 | 142 | 177 | 283 | 340 |
Fe20 | 94 | 146 | 177 | 248 | 272 |
Catalyst | Weight Loading [wt%] | m (Fe) [mg] | n (Fe(acac)3) [mmol] | m (γ-Al2O3) [g] |
---|---|---|---|---|
Fe01 | 1 | 20 | 0.358 | 1.98 |
Fe025 | 2.5 | 50 | 0.895 | 1.95 |
Fe05 | 5 | 100 | 1.79 | 1.90 |
Fe10 | 10 | 200 | 3.58 | 1.80 |
Fe20 | 20 | 400 | 7.16 | 1.60 |
Energy [eV] | Step Size | Time per Point [s] |
---|---|---|
6962–7062 | 5 eV | 0.2 |
7062–7092 | 3 eV | 0.2 |
7092–7142 | 0.5 eV | 0.2 |
7142–8112 | 0.5 Å−1 | 0.2 |
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Schlicher, S.; Prinz, N.; Bürger, J.; Omlor, A.; Singer, C.; Zobel, M.; Schoch, R.; Lindner, J.K.N.; Schünemann, V.; Kureti, S.; et al. Quality or Quantity? How Structural Parameters Affect Catalytic Activity of Iron Oxides for CO Oxidation. Catalysts 2022, 12, 675. https://doi.org/10.3390/catal12060675
Schlicher S, Prinz N, Bürger J, Omlor A, Singer C, Zobel M, Schoch R, Lindner JKN, Schünemann V, Kureti S, et al. Quality or Quantity? How Structural Parameters Affect Catalytic Activity of Iron Oxides for CO Oxidation. Catalysts. 2022; 12(6):675. https://doi.org/10.3390/catal12060675
Chicago/Turabian StyleSchlicher, Steffen, Nils Prinz, Julius Bürger, Andreas Omlor, Christian Singer, Mirijam Zobel, Roland Schoch, Jörg K. N. Lindner, Volker Schünemann, Sven Kureti, and et al. 2022. "Quality or Quantity? How Structural Parameters Affect Catalytic Activity of Iron Oxides for CO Oxidation" Catalysts 12, no. 6: 675. https://doi.org/10.3390/catal12060675