The role of alkali metal ions on hydrothermal stability of Cu/SSZ-13 NH3-SCR catalysts

The role of alkali metal ions on hydrothermal stability of Cu/SSZ-13 NH3-SCR catalysts
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碱金属离子对Cu/SSZ-13 NH3-SCR催化剂水热稳定性的影响

DOI:
10.1016/j.cattod.2019.06.074
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发表时间:
2020-09
期刊:
影响因子:
5.3
通讯作者:
Xue Kang
Xue Kang
中科院分区:
化学2区
文献类型:
--
作者:
Chen Wang;Wenjun Yan;Zhixin Wang;Zexiang Chen;Jianqiang Wang;Jun Wang;Jiaming Wang;Meiqing Shen;Xue Kang

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Cu/SSZ-13 被认为是 NH3-SCR 催化剂的良好候选者。然而,在现实世界中,Cu/SSZ-13不可避免地会暴露于碱金属沉积和水热老化中,因此,本工作研究了碱离子(Na+和K+)中毒对Cu/SSZ-13水热稳定性的作用。 Cu/SSZ-13催化剂在600℃下采用不同碱含量负载量或在低碱金属负载量下采用不同水热温度进行处理。与水热老化下未中毒的Cu/SSZ-13催化剂不同,引入的碱离子削弱了Cu/SSZ-13的水热稳定性,使得中毒催化剂的SCR性能较差。 H2-TPR 结果表明碱离子的存在导致更多的铜离子转化为氧化铜物质,并且转化程度随着碱含量和老化温度的增加而增加。此外,XRD结果表明,在高碱离子含量或高老化温度下,CHA骨架崩溃,同时形成SiO2和CuAlOx物质。此外,由于水合直径小,结合能力强,钾总是表现出严重的失活。我们的研究表明,柴油应注意控制汽车产品中碱离子(尤其是K+)的含量以及后处理应用中的操作温度。
Cu/SSZ-13 has considered being a good candidate for NH3-SCR catalysts. However, in real world, Cu/SSZ-13 inevitably expose to alkali metals deposit and hydrothermal aging, and hence, the role of alkali ions (Na+and K+) poisoning on the hydrothermal stability of Cu/SSZ-13 was investigated in this work. The Cu/SSZ-13 catalyst was treated with different loadings of alkali content at 600 °C or different hydrothermal temperatures at low alkali metal loading. Different from non-poisoned Cu/SSZ-13 catalysts under hydrothermal aging, the introduced alkali ions weaken the hydrothermal stability of Cu/SSZ-13 and make poisoned catalysts have inferior SCR performance. H2-TPR results demonstrate the presence of alkali ions lead to more copper ions transform to copper oxides species and the extents of transformation increase as the alkali contents and aging temperature increasing. Moreover, XRD results prove that the CHA framework collapse and, simultaneously, SiO2and CuAlOxspecies form under high contents of alkali ions or high aging temperature. Besides, potassium invariably shows the severe deactivation because of a small hydrated diameter and strong binding ability. Our study reveals that diesel should pay attention to control the contents of alkali ions, especially for K+, in automotive products and the operating temperature in after-treatment applications.
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