Simultaneous removal of NO and CO over Ni-Ce bifunctional catalyst supported by modified activated coke at oxygen-rich condition
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摘要: 采用等体积浸渍法制备的改性活性焦（AC-N）负载Ni-Ce过渡金属催化剂可同时催化氨选择性催化还原（NH3-SCR）反应和CO氧化反应，实现低温富氧条件下NO和CO的一体化脱除。Ni-Ce/AC-N催化剂在175–250 ℃可实现NO和CO的高效转化，NO和CO转化率在175−250 ℃均高于95%。硝酸改性后活性焦载体与金属组分之间有更强烈的相互作用，有利于活性组分在催化剂表面更好的分散，提高催化剂的比表面积和氧化还原能力；Ni、Ce之间存在协同作用，使得催化剂表面出现更多的Ni2+和 Ce3+，有利于催化活性提高。Abstract: The modified activated coke (AC-N) supported Ni-Ce transition metal catalyst prepared by incipient-wetness impregnation method can simultaneously catalyze the ammonia selective catalytic reduction (NH3-SCR) reaction and CO oxidation reaction, realizing the removal of NO and CO under low temperature and oxygen-rich conditions. The Ni-Ce /AC-N catalyst can achieve high-efficiency conversion of NO and CO at 175–250 ℃, and the conversion rates of NO and CO are both above 95% in this temperature range. After modified by nitric acid, the active coke support has a stronger interaction with metal components, which is conducive to better dispersion of the active components on the catalyst surface, and improves the specific surface area and redox capacity of the catalyst. The synergistic effect between Ni and Ce results in more Ni2+ and Ce3+ species on the catalyst surface, which is beneficial to the improvement of catalytic activity.
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Key words:
- SCR /
- CO /
- catalytic oxidation /
- transition metal /
- modified active coke
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图 1 AC、AC-N、Ni/AC、Ni/AC-N、Ni-Ce/AC、Ni-Ce/AC-N 催化剂NO、CO转化率和N2选择性
Figure 1 NO, CO conversion and N2 selectivity AC, AC-N, Ni/AC, Ni/AC-N, Ni-Ce/AC, Ni-Ce/AC-N (a): SCR activities; (b): CO oxidation activities; (c): N2 selectivity
图 3 催化剂AC-N、Ni/AC、Ni/AC-N、Ni-Ce/AC、Ni-Ce/AC-N的XRD谱图
Figure 3 XRD patterns of AC, AC-N, Ni/AC, Ni/AC-N, Ni-Ce/AC and Ni-Ce/AC-N
图 4 AC、AC-N、Ni/AC、Ni/AC-N、Ni-Ce/AC、Ni-Ce/AC-N催化剂红外光谱谱图
Figure 4 Infrared spectra of AC, AC-N, Ni/AC, Ni/AC-N, Ni-Ce/AC and Ni-Ce/AC-N
图 5 AC、AC-N、Ni/AC、Ni/AC-N、Ni-Ce/AC、Ni-Ce/AC-N催化剂H2-TPR谱图
Figure 5 H2-TPR profiles of AC, AC-N, Ni/AC, Ni/AC-N, Ni-Ce/AC and Ni-Ce/AC-N
图 6 Ni 2p、Ce 3d和O 1s轨道 XPS谱图
Figure 6 XPS profiles of Ni 2p (a), Ce 3d (b) and O 1s (c)
表 1 催化剂的织构性质
Table 1 Textural properties of all catalyst samples
Sample SBET /(m2·g−1) vtotal /(mL·g−1) dmean /nm AC 201.5 0.11 0.8 AC-N 242.6 0.13 0.4 Ni/AC 234.1 0.14 0.4 Ni/AC-N 271.2 0.13 0.4 Ni-Ce/AC 224.3 0.12 0.4 Ni-Ce/AC-N 280.4 0.17 0.4 
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表 2 元素价态的相对含量
Table 2 Relative content of element valence state
Sample Components/% Ni2+ Ce3+ Oβ Ni/AC 79.85 59.45 Ni/AC-N 82.65 69.54 Ni-Ce/AC 85.78 17.69 55.22 Ni-Ce/AC-N 88.42 21.07 61.01
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