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Deactivation of Cu-SSZ-13 by SO2 exposure under SCR conditions

机译：失活的Cu-SSZ-13二氧化硫接触下可控硅的条件

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A deactivation study of Cu-SSZ-13 has been conducted using SO2 exposure under SCR conditions and examining its effect on different reactions involving NH3-SCR. Several reactions, including NH3 storage/TPD, NO/NH3 oxidation, standard SCR, fast SCR and SCR with 75% NO2, as well as NH3-NO2 storage/TPD, were investigated at a temperature range of 100-400 degrees C after exposing the catalyst to 30 ppm SO2 under SCR conditions at 300 degrees C for 90 min. The catalyst was characterized using XRD, BET, ICP-SFMS and H-2-TPR. The BET surface area and pore volume decreased after the sulfur treatment presumably due to blocking by sulfur and/or ammonium-sulfur species. It was found that sulfur was not uniformly deposited along the monolith channel. The deposition occurred from the inlet towards the outlet, as evident from ICP-SFMS measurements. Part of the sulfur was removed after an SCR experiment up to 400 degrees C. However, this removal was observed only in the inlet half of the sample and not in the outlet. Ammonia TPD experiments revealed that the sulfur poisoning resulted in additional sites that were capable of adsorbing ammonia, resulting in increased ammonia storage. Moreover, standard SCR was significantly deactivated by SO2 poisoning under SCR conditions. Due to the site-blocking effect of the ammonium-sulfur species, fewer copper sites are likely available for the redox SCR cycle. Furthermore, the effect of sulfur poisoning on NH3 oxidation and NO2-SCR as well as N2O production in various SCR reactions were observed. Finally, it was found that the conditions for the sulfur poisoning were critical in which SO2 deactivation under SCR conditions (NH3 + NO+ O-2 + H2O) was more severe compared to SO2 poisoning in O-2 + H2O alone.
机译：失活研究Cu-SSZ-13使用二氧化硫暴露在可控硅的条件下进行对不同的反应,考察其影响涉及NH3-SCR。NH3 /存储信息,没有/氨氧化,标准的可控硅,快速可控硅NO2和可控硅75%,以及NH3-NO2存储/信息,研究了温度暴露后的100 - 400摄氏度范围可控硅条件下催化剂30 ppm二氧化硫300摄氏度90分钟的催化剂使用XRD,打赌,ICP-SFMS和H-2-TPR。硫磺治疗后可能下降由于硫和/或ammonium-sulfur阻塞物种。沿着庞然大物通道均匀沉积。从入口向沉积发生出口,从ICP-SFMS明显测量。后一个SCR实验400摄氏度。然而,这只观察去除进口样品,而不是出口的一半。氨一系列实验表明硫中毒导致更多的网站能够吸附氨,导致增加氨存储。明显释放二氧化硫中毒可控硅的条件下。影响ammonium-sulfur物种,更少铜的网站很可能用于氧化还原可控硅周期。在氨氧化和NO2-SCR以及中毒一氧化二氮生产各种SCR反应观察到。硫中毒的条件是至关重要的二氧化硫在可控硅条件下失活(NH3 +不+ 0 2 + H2O)相比是更严重的二氧化硫中毒在0 2 + H2O。

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