In Situ Regeneration and Deactivation of Co-Zn/H-Beta Catalysts in Catalytic Reduction of NOx with Propane

In Situ Regeneration and Deactivation of Co-Zn/H-Beta Catalysts in Catalytic Reduction of NOx with Propane
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Co-Zn/H-Beta 催化剂在丙烷催化还原 NOx 中的原位再生和失活

DOI:
10.3390/catal9010023
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发表时间:
2018-12
期刊:
影响因子:
3.9
通讯作者:
Chao Shen
Chao Shen
中科院分区:
化学3区
文献类型:
--
作者:
Hua Pan;Dongmei Xu;Chi He;Chao Shen

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研究了Co-Zn/H-Beta催化剂在C3H8还原NOx过程中的再生和失活行为。Co-Zn/ h - β在10 vol.% H2O的存在下表现出良好的耐水性。然而,在SO2的存在下,N2产率明显下降。在C3H8还原NO反应中,表面硫酸盐和焦炭的形成使Co-Zn/H-Beta的表面积减小,孔隙结构堵塞,活性位点的可用性降低。空气氧化- H2还原再生催化剂的活性高于空气氧化- H2还原再生催化剂的活性。不同再生温度下空气氧化- H2还原再生催化剂的最佳再生温度为550℃。优化后的再生工艺可使中毒催化剂的织构性能恢复到新鲜催化剂的水平。空气氧化+ H2还原再生工艺可以从硫酸盐中恢复钴和锌的活性位点,并消除中毒催化剂上的积炭。将空气氧化- H2还原再生途径概括为空气氧化先脱除焦炭,H2最终还原硫酸盐。
Regeneration and deactivation behaviors of Co-Zn/H-Beta catalysts were investigated in NOx reduction with C3H8. Co-Zn/H-Beta exhibited a good water resistance in the presence of 10 vol.% H2O. However, there was a significant drop off in N2 yield in the presence of SO2. The formation of surface sulfate and coke decreased the surface area, blocked the pore structure, and reduced the availability of active sites of Co-Zn/H-Beta during the reaction of NO reduction by C3H8. The activity of catalyst regenerated by air oxidation followed by H2 reduction was higher than that of catalyst regenerated by H2 reduction followed by air oxidation. Among the catalysts regenerated by air oxidation followed by H2 reduction with different regeneration temperatures, the optimal regeneration temperature was 550 °C. The textural properties of poisoned catalysts could be restored to the levels of fresh catalysts by the optimized regeneration process. The regeneration process of air oxidation followed by H2 reduction could recover the active sites of cobalt and zinc species from sulfate species, as well as eliminate coke deposition on poisoned catalysts. The regeneration pathway of air oxidation followed by H2 reduction is summarized as initial removal of coke by air oxidation and final reduction of the sulfate species by H2.
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