Unraveling the nature of sulfur poisoning on Cu/SSZ-13 as a selective reduction catalyst
Unraveling the nature of sulfur poisoning on Cu/SSZ-13 as a selective reduction catalyst
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揭示 Cu/SSZ-13 作为选择性还原催化剂的硫中毒本质
DOI：
10.1016/j.jtice.2020.12.033
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发表时间：
2021
影响因子：
5.7
通讯作者：
Meiqing Shen
中科院分区：
文献类型：
--
作者：
Chen Wang;Zexiang Chen;Jun Wang;Jianqiang Wang;Meiqing Shen
为了研究用于通过氨选择性催化还原（NH3-SCR）去除NOx的Cu/SSZ-13催化剂的硫酸盐中毒，将它们在存在和不存在NH3的情况下在不同温度下暴露于SO2。进行标准物理化学表征和密度泛函理论计算，以探讨催化剂上形成的硫酸盐物质的性质以及相应的影响。结果表明，硫酸盐中毒对催化剂菱沸石结构影响不大，但形成的硫酸盐物质堵塞了Cu/SSZ-13孔道。对于纯 SO2 的硫酸化，会形成硫酸氢铜，其含量随硫酸化温度的升高而增加。然而，在 NH3 存在的情况下，形成的主要硫酸盐是硫酸氢铵 (~80%)。此外，由于硫酸氢铵形成困难，硫酸化温度越高，总硫酸盐含量越低。无论形成的硫酸盐种类如何，中毒都会导致活性位点的可用性降低，从而导致氮氧化物转化率降低。重要的是，由于Z-Cu(OH)+上的硫酸氢铜和硫酸氢铵可以相互转化，我们的研究表明，使用NH3促进硫酸氢铜向硫酸氢铵的转化是提高硫酸化Cu/SSZ-13回收效果的可行方法。
In order to investigate sulfate poisoning of Cu/SSZ-13 catalysts used for NOxremoval by selective catalytic reduction with ammonia (NH3-SCR), they were exposed to SO2at different temperatures in the presence and absence of NH3. Standard physicochemical characterization and density functional theory calculations were performed to probe the nature of the sulfate species formed on the catalyst and the corresponding effects. The results showed that sulfate poisoning has little effect on the chabazite structure of the catalyst, but the sulfate species formed blocks the Cu/SSZ-13 pores. For sulfation with pure SO2, copper bisulfate forms and its content increases with sulfation temperature. However, in the presence of NH3, the major sulfate formed is ammonium bisulfate (~80%). Moreover, the total sulfate contents are lower for higher sulfation temperatures because of difficulties in ammonium bisulfate formation. Regardless of the kind of sulfate species formed, the poisoning leads to lower availability of active sites, causing inferior NOx conversion. Importantly, as copper bisulfate and ammonium bisulfate on Z-Cu(OH)+are interconvertible, our study reveals that using NH3to promote the transformation from copper bisulfate to ammonium bisulfate is a viable method to improve the recovery effect of sulfated Cu/SSZ-13.
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