Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (3): 396-408.DOI: 10.1016/S1872-2067(20)63657-9
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Xiaohui Feng, Rui Liu, Xianglan Xu, Yunyan Tong, Shijing Zhang, Jiacheng He, Junwei Xu, Xiuzhong Fang, Xiang Wang*()
Received:
2020-05-11
Accepted:
2020-06-20
Online:
2021-03-18
Published:
2021-01-23
Contact:
Xiang Wang
About author:
*Tel:+86-15979149877;E-mail:xwang23@ncu.edu.cnSupported by:
Xiaohui Feng, Rui Liu, Xianglan Xu, Yunyan Tong, Shijing Zhang, Jiacheng He, Junwei Xu, Xiuzhong Fang, Xiang Wang. Stable CuO/La2Sn2O7 catalysts for soot combustion: Study on the monolayer dispersion behavior of CuO over a La2Sn2O7 pyrochlore support[J]. Chinese Journal of Catalysis, 2021, 42(3): 396-408.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63657-9
Sample | CuO loading a (wt%) | Surface area b (m2 g-1) | Average pore size c (nm) | Average pore volume c (cm3 g-1) |
---|---|---|---|---|
La2Sn2O7 | — | 17.5 | 10.2 | 0.057 |
1% CuO/La2Sn2O7 | 0.9 | 16.5 | 10.4 | 0.049 |
2% CuO/La2Sn2O7 | 1.9 | 15.9 | 10.3 | 0.042 |
3% CuO/La2Sn2O7 | 2.9 | 15.5 | 10.4 | 0.039 |
4% CuO/La2Sn2O7 | 4.0 | 15.1 | 10.6 | 0.037 |
5% CuO/La2Sn2O7 | 4.9 | 14.9 | 11.1 | 0.034 |
6% CuO/La2Sn2O7 | 6.0 | 14.7 | 11.5 | 0.031 |
7% CuO/La2Sn2O7 | 7.1 | 10.1 | 11.4 | 0.031 |
8% CuO/La2Sn2O7 | 8.1 | 9.6 | 11.7 | 0.030 |
9% CuO/La2Sn2O7 | 9.1 | 7.6 | 12.9 | 0.030 |
Table 1 Textural properties measured by N2 sorption.
Sample | CuO loading a (wt%) | Surface area b (m2 g-1) | Average pore size c (nm) | Average pore volume c (cm3 g-1) |
---|---|---|---|---|
La2Sn2O7 | — | 17.5 | 10.2 | 0.057 |
1% CuO/La2Sn2O7 | 0.9 | 16.5 | 10.4 | 0.049 |
2% CuO/La2Sn2O7 | 1.9 | 15.9 | 10.3 | 0.042 |
3% CuO/La2Sn2O7 | 2.9 | 15.5 | 10.4 | 0.039 |
4% CuO/La2Sn2O7 | 4.0 | 15.1 | 10.6 | 0.037 |
5% CuO/La2Sn2O7 | 4.9 | 14.9 | 11.1 | 0.034 |
6% CuO/La2Sn2O7 | 6.0 | 14.7 | 11.5 | 0.031 |
7% CuO/La2Sn2O7 | 7.1 | 10.1 | 11.4 | 0.031 |
8% CuO/La2Sn2O7 | 8.1 | 9.6 | 11.7 | 0.030 |
9% CuO/La2Sn2O7 | 9.1 | 7.6 | 12.9 | 0.030 |
Fig. 4. Soot combustion activity on the CuO/La2Sn2O7 catalysts under tight contact conditions. TPO profiles (a) and stability tests (b) of 4% CuO/La2Sn2O7 over five continuous TPO cycles.
Sample | Ti (°C) | Tp (°C) | Tc (°C) | ΔTi-p (°C) | SCO2 (%) |
---|---|---|---|---|---|
Soot | 530 | 640 | 690 | 110 | 68 |
La2Sn2O7 | 425 | 525 | 600 | 100 | 89 |
1% CuO/La2Sn2O7 | 420 | 515 | 590 | 95 | 92 |
2% CuO/La2Sn2O7 | 420 | 500 | 580 | 80 | 93 |
3% CuO/La2Sn2O7 | 400 | 490 | 565 | 90 | 94 |
4% CuO/La2Sn2O7 | 395 | 460 | 535 | 65 | 97 |
5% CuO/La2Sn2O7 | 395 | 470 | 540 | 75 | 96 |
6% CuO/La2Sn2O7 | 400 | 470 | 545 | 70 | 96 |
7% CuO/La2Sn2O7 | 400 | 475 | 550 | 75 | 95 |
8% CuO/La2Sn2O7 | 405 | 475 | 550 | 70 | 95 |
9% CuO/La2Sn2O7 | 405 | 480 | 555 | 75 | 95 |
Table 2 Soot combustion activity on the CuO/La2Sn2O7 catalysts.
Sample | Ti (°C) | Tp (°C) | Tc (°C) | ΔTi-p (°C) | SCO2 (%) |
---|---|---|---|---|---|
Soot | 530 | 640 | 690 | 110 | 68 |
La2Sn2O7 | 425 | 525 | 600 | 100 | 89 |
1% CuO/La2Sn2O7 | 420 | 515 | 590 | 95 | 92 |
2% CuO/La2Sn2O7 | 420 | 500 | 580 | 80 | 93 |
3% CuO/La2Sn2O7 | 400 | 490 | 565 | 90 | 94 |
4% CuO/La2Sn2O7 | 395 | 460 | 535 | 65 | 97 |
5% CuO/La2Sn2O7 | 395 | 470 | 540 | 75 | 96 |
6% CuO/La2Sn2O7 | 400 | 470 | 545 | 70 | 96 |
7% CuO/La2Sn2O7 | 400 | 475 | 550 | 75 | 95 |
8% CuO/La2Sn2O7 | 405 | 475 | 550 | 70 | 95 |
9% CuO/La2Sn2O7 | 405 | 480 | 555 | 75 | 95 |
Samples | O2-TPD | Soot-TPR | ||
---|---|---|---|---|
Oxygen from α peak (μmol g-1) | Oxygen from β peak (μmol g-1) | Active oxygen (μmol g-1) | Oxygen uptake from α peak (a.u.) | |
La2Sn2O7 | 3.56 | — | 3.56 | 12.3 |
1% CuO/La2Sn2O7 | 4.27 | 11.41 | 15.68 | 25.2 |
3% CuO/La2Sn2O7 | 4.70 | 15.51 | 20.21 | 38.5 |
4% CuO/La2Sn2O7 | 5.70 | 35.21 | 40.91 | 100.0 |
5% CuO/La2Sn2O7 | 7.98 | 29.14 | 37.12 | 82.9 |
7% CuO/La2Sn2O7 | 5.56 | 27.47 | 33.03 | 78.4 |
9% CuO/La2Sn2O7 | 6.13 | 25.24 | 31.37 | 72.4 |
Table 3 Quantified O2-TPD and soot-TPR results for the CuO/La2Sn2O7 catalysts.
Samples | O2-TPD | Soot-TPR | ||
---|---|---|---|---|
Oxygen from α peak (μmol g-1) | Oxygen from β peak (μmol g-1) | Active oxygen (μmol g-1) | Oxygen uptake from α peak (a.u.) | |
La2Sn2O7 | 3.56 | — | 3.56 | 12.3 |
1% CuO/La2Sn2O7 | 4.27 | 11.41 | 15.68 | 25.2 |
3% CuO/La2Sn2O7 | 4.70 | 15.51 | 20.21 | 38.5 |
4% CuO/La2Sn2O7 | 5.70 | 35.21 | 40.91 | 100.0 |
5% CuO/La2Sn2O7 | 7.98 | 29.14 | 37.12 | 82.9 |
7% CuO/La2Sn2O7 | 5.56 | 27.47 | 33.03 | 78.4 |
9% CuO/La2Sn2O7 | 6.13 | 25.24 | 31.37 | 72.4 |
Fig. 8. In situ DRIFTS spectra showing the effects on the surface oxygen sites on 4% CuO/La2Sn2O7 at 400 °C after pretreatment at 400 °C in an Ar feed for 1 h. (a) In a 10% O2/Ar feed; (b) in a 10% H2/Ar feed; (c) after re-exposure to the 10% O2/Ar feed.
Sample | O 1s binding energy and relative amount (%) | (O2- + O22-)/O2- ratio | ||
---|---|---|---|---|
O2- | O22- | O2- | ||
1% CuO/La2Sn2O7 | 532.8/7.6 | 531.5/43.5 | 529.8/48.9 | 1.05 |
3% CuO/La2Sn2O7 | 532.9/19.7 | 531.6/40.4 | 529.8/39.9 | 1.50 |
4% CuO/La2Sn2O7 | 532.7/16.2 | 531.5/54.4 | 529.7/29.4 | 2.40 |
5% CuO/La2Sn2O7 | 532.6/18.6 | 531.5/49.9 | 529.9/31.5 | 2.17 |
7% CuO/La2Sn2O7 | 532.8/21.3 | 531.4/46.2 | 529.7/32.5 | 2.08 |
9% CuO/La2Sn2O7 | 532.7/13.3 | 531.4/53.8 | 529.8/32.9 | 2.04 |
Table 4 Quantified XPS O 1s results for the CuO/La2Sn2O7 catalysts.
Sample | O 1s binding energy and relative amount (%) | (O2- + O22-)/O2- ratio | ||
---|---|---|---|---|
O2- | O22- | O2- | ||
1% CuO/La2Sn2O7 | 532.8/7.6 | 531.5/43.5 | 529.8/48.9 | 1.05 |
3% CuO/La2Sn2O7 | 532.9/19.7 | 531.6/40.4 | 529.8/39.9 | 1.50 |
4% CuO/La2Sn2O7 | 532.7/16.2 | 531.5/54.4 | 529.7/29.4 | 2.40 |
5% CuO/La2Sn2O7 | 532.6/18.6 | 531.5/49.9 | 529.9/31.5 | 2.17 |
7% CuO/La2Sn2O7 | 532.8/21.3 | 531.4/46.2 | 529.7/32.5 | 2.08 |
9% CuO/La2Sn2O7 | 532.7/13.3 | 531.4/53.8 | 529.8/32.9 | 2.04 |
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