Catalytic performance and hydrothermal stability of Cu/SAPO-34 catalyst in the selective catalytic oxidation of NH3
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摘要: 采用浸渍法制备了一系列不同铜含量的Cu/SAPO-34催化剂，考察了该系列催化剂上NH3选择性催化氧化反应性能（NH3-SCO）。实验结果表明，10%-Cu/SAPO-34催化剂在300 ℃温度下具有100%的NH3去除率，且其氮气选择性大于90%。与此同时，通过XRD、BET、UV-vis、H2-TPR和XPS等表征分析结果表明，高度分散的CuO是Cu/SAPO-34催化剂的主要活性组分。对10%-Cu/SAPO-34催化剂进行水热处理后，催化剂低温活性明显提高，催化剂的N2选择性在325 ℃急剧下降。这是由于水热处理导致一定数量的铜物种发生迁移并且形成了更稳定的铜物种引起。SAPO-34的骨架结构遭到一定程度的破坏。Abstract: A series of Cu/SAPO-34 catalysts for ammonia selective catalytic oxidation (NH3-SCO) were prepared by impregnation method. The results of activity test indicated that the NH3 conversion over 10%-Cu/SAPO-34 catalyst was nearly 100% at 300℃ and N2 selectivity was more than 90% in the range of test temperature. Meanwhile, the characterization results of XRD, BET, UV-vis, H2-TPR and XPS showed that the highly dispersed CuO species in Cu/SAPO-34 catalyst were the main active component. Furthermore, the aged 10%-Cu/SAPO-34 catalyst performed better NH3-SCO activity at low temperature, while the N2 selectivity dramatically decreased at 325℃, SAPO-34 zeolite crystallinity would deteriorate under hydrothermal treatment.
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Key words:
- NH3-SCO /
- CuO /
- SAPO-34 /
- hydrothermal treatment
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图 1 不同催化剂的NH3转化率(a)，NO生成量(b), NO2生成量(c)，N2O生成量(d)和N2选择性(e)
Figure 1 NH3 conversion (a), NOproduction (b), NO2production (c), N2Oproduction (d) and N2 selectivity (e) of different catalysts
图 5 新鲜和老化催化剂的NH3转化率、NOx生成量和N2选择性
Figure 5 NH3 conversion, NOx production and N2 selectivity of catalysts before and after aging
图 7 水热处理前后Cu/SAPO-34催化剂的Cu 2p XPS
Figure 7 Cu 2p XPS of Cu/SAPO-34 catalysts before and after hydrothermal aging
图 8 水热处理前后催化剂的UV-vis谱图
Figure 8 UV-vis results of the catalysts before and after hydrothermal aging
图 9 水热处理前后催化剂的H2-TPR谱图
Figure 9 H2-TPR profiles of the catalysts before and after hydrothermal aging
表 1 不同催化剂的比表面积和孔容
Table 1 BET surface area and pore volume of different catalysts
Sample ABET/(m2·g-1) Pore volume v/(cm3·g-1) SAPO-34 210 0.1121 5%-Cu/SAPO-34 186 0.1437 10%-Cu/SAPO-34 166 0.1423 15%-Cu/SAPO-34 158 0.1464 20%-Cu/SAPO-34 141 0.1135 25%-Cu/SAPO-34 117 0.1074 30%-Cu/SAPO-34 128 0.1028 
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